On the April 4, 2008 episode of SmackDown, she made her main roster debut, as a villain, when she came out of the crowd to aid Victoria in an attack against Michelle McCool and Cherry, forming an alliance with her in the process. On the April 11, 2008 episode of SmackDown!, she introduced herself as the daughter of Jim Neidhart under the name Natalya Neidhart, accompanying Victoria to her match against Michelle McCool. Two weeks later on SmackDown she made her televised in-ring debut, under the shortened ring name Natalya, defeating Cherry with her uncle's submission move the "sharpshooter". At the Backlash pay–per–view on April 27, Natalya teamed up with Victoria, Beth Phoenix, Jillian Hall, Layla and Melina to defeat Mickie James, Maria Kanellis, Ashley, Michelle McCool, Cherry and Kelly Kelly in a 12-Diva tag team match. On the May 2 episode of SmackDown, Victoria and Natalya defeated McCool and Cherry. On the June 6 episode of SmackDown, SmackDown General Manager Vickie Guerrero introduced the Divas Championship, and that same night the Divas competed in a Golden Dreams match to qualify for the championship match at The Great American Bash. Natalya won and advanced to the Bash, but lost the championship match to Michelle McCool.
Natalya and Victoria started a feud with the debuting Brie Bella, after Victoria lost to her on the August 29 episode of SmackDown. On the September 26 episode of SmackDown, Victoria and Natalya lost to Maria and Brie. On the October 31 episode of SmackDown, Natalya teamed up with Victoria and Maryse during a Divas Halloween costume tag team match in a losing effort to Michelle McCool, Maria and Brie. On the November 7 episode of SmackDown, Natalya accompanied Victoria to her match against Brie, where she was once again defeated. Post-match, Brie ran under the ring to escape from Natalya and Victoria, but they both reached under the ring for her, pulling her and her twin sister Nicole out. The twins then attacked them and celebrated afterward. On the November 21 episode of SmackDown, Victoria teamed up with Natalya in a losing effort to The Bella Twins. At Survivor Series, Natalya competed in a 5-on-5 Survivor Series elimination match apart of Team Smackdown where her team lost to Team Raw. On the November 28 episode of SmackDown, Victoria teamed up with Natalya and Maryse to defeat the Bella Twins and Michelle McCool, before the feud ended. Followed this, her association with Victoria also ended after she retired from the company on the January 16, 2009 episode of SmackDown. At Armageddon, Natalya, Jillian Hall, Victoria and Maryse lost to Maria, Kelly Kelly, Mickie James, and Michelle McCool in an Eight-Diva Santa's Little Helper tag team match.
While still a member of the SmackDown brand, she made her debut for the ECW brand, via the talent exchange agreement, on February 10, 2009, managing her real life boyfriend Tyson Kidd. In her ECW in-ring debut, on the March 3 episode, Natalya defeated Alicia Fox. On April 5, Neidhart competed in a Divas battle royal at WrestleMania XXV, but the match was won by Santina Marella. On April 15 Natalya was made an official member of the ECW brand, when she was drafted there as part of the 2009 Supplemental Draft. On the May 13 episode of ECW, Kidd and Natalya were joined by her real-life cousin David Hart Smith, forming The Hart Dynasty, although it was originally called The Hart Trilogy.
On June 29, 2009, Natalya was traded back to SmackDown along with the other members of The Hart Dynasty. Natalya's first match back for the brand was in a six-person mixed tag team match on the July 17 episode, when The Hart Dynasty defeated Cryme Tyme (JTG and Shad Gaspard) and Eve Torres. Natalya, Kidd, and Smith went on to feud with Torres and Cryme Tyme, with Natalya also facing Torres in singles matches and tag team matches involving other Divas. Natalya was on the winning team when the SmackDown Divas defeated the Raw Divas at the Bragging Rights pay-per-view in October. On December 4, Natalya lost in a triple threat match to determine to number one contender for the WWE Women's Championship after she was pinned by Mickie James. The match also involved Beth Phoenix.
Natalya, along with the other Hart Dynasty members, appeared at WrestleMania XXVI, helping her uncle Bret Hart during his match against Vince McMahon, turning them into faces as a result. On April 26, The Hart Dynasty won the Unified WWE Tag Team Championship from The Miz and The Big Show. The following day, as part of the 2010 WWE Supplemental Draft, Natalya was drafted to the Raw brand, along with Kidd and Smith. On the May 24, 2010, episode of Raw, all three members of The Hart Dynasty were attacked by The Usos (Jimmy and Jey Uso) and Tamina, who were making their debuts. This provoked a feud between the trios, with The Hart Dynasty attacking The Usos and Tamina the following week in retaliation. At the Fatal 4-Way pay-per-view in June, Natalya and The Hart Dynasty defeated Tamina and The Uso brothers in a six-person mixed tag team match, when Natalya pinned Tamina following a discus clothesline. At the next pay-per-view, Money in the Bank, Natalya helped The Hart Dynasty to retain the championship against The Usos by stopping Tamina from interfering in the match, ending the feud. In September, at Night of Champions, The Hart Dynasty lost the Tag Team Championship in a Tag Team Turmoil match. After a failed attempt to regain the championship, in which Kidd was pushed off balance during their double-team Hart Attack move, Kidd and Smith began to have a falling out with one another.
This culminated on the November 15 episode of Raw, when Kidd refused to tag in and attacked Smith during a match for the WWE Tag Team Championship against The Nexus (Justin Gabriel and Heath Slater), resulting in Kidd became a heel once again. Smith defeated Kidd in a singles match on the November 25 episode of WWE Superstars. Afterward, Smith offered to shake Kidd's hand, but Kidd refused and instead slapped him across the face. On the following episode of Raw, Kidd defeated Smith in a rematch, with this officially ending the alliance as a team.
Natalya started her singles competition run, on the September 27 episode of Raw, when she won a battle royal to become the number one contender to the WWE Unified Divas Championship, and began feuding with self-professed co-Divas Champions Lay-Cool (Michelle McCool and Layla). At the Hell in a Cell pay-per-view on October 3, she defeated Michelle McCool via disqualification in a match for the championship, which meant that McCool retained the championship. She received another championship match three weeks later at the Bragging Rights pay-per-view, where she lost to Layla after McCool interfered. On November 1, she once again became number one contender to the Unified Divas Championship after defeating McCool in a non-title match.
At the Survivor Series pay-per-view on November 21, Natalya defeated McCool and Layla in a two-on-one handicap match to win the WWE Divas Championship for the first time. After the match she was attacked by Lay-Cool until Beth Phoenix came to her aid, with the pair forming an alliance. At the TLC: Tables, Ladders & Chairs pay-per-view in December, Natalya and Phoenix defeated Lay-Cool in the first Diva's Tag Team Tables match in WWE history. Natalya was scheduled to defend her championship against Lay-Cool in a two-on-one handicap match at the Royal Rumble, but the match was changed to a fatal four-way, also involving Eve. Eve went on to pin Layla and become the new Divas Champion ending Natalya's reign at 70 days.
On April 26, Natalya was drafted back to the SmackDown brand as part of the 2011 supplemental draft. In her return match for the brand, she unsuccessfully challenged Brie Bella for the Divas Championship. In May, Natalya began acting as the on-screen mentor to The Chickbusters (AJ and Kaitlyn), giving them advice and managing them during their matches. Natalya, AJ, and Kaitlyn feuded with Alicia Fox, Tamina, and Rosa Mendes throughout 2011.
On the August 1, 2011, episode of Raw, she competed in a battle royal to determinate the number one contender to Kelly Kelly's Divas Championship at SummerSlam, which was won by Beth Phoenix. Post-match, she turned villainous by attacking Kelly, and stating "[her] days as the perky, cute, blonde little bimbo were officially over", four days later on SmackDown, Natalya defeated AJ before turning on her protégé, attacking her and declaring war on the "perky little princesses" that comprised the rest of the Divas division. As part of the storyline, she aligned herself with Phoenix, and the pair dubbed themselves "The Divas of Doom", defeating The Chickbusters the following week. Throughout September, The Divas of Doom feuded with The Chickbusters on SmackDown, while feuding with Kelly Kelly and Eve Torres on Raw.
Natalya accompanied Phoenix to her Divas Championship match at the SummerSlam pay-per-view against Kelly Kelly, who was accompanied by Eve Torres, but she failed to win the match. On the September 19 episode of Raw, the Divas of Doom lost a tag team match to Kelly and Torres after Eve pinned Natalya for the win. On the September 26 episode of Raw, Phoenix pinned Kelly Kelly in a tag team match and granted her a new match for Kelly's WWE Divas Championship. Four days later on SmackDown, Natalya lost a match to Kelly. Post-match, Phoenix jumped into the ring and delivered a 'Glam Slam' on Kelly, then Natalya applied and debuted their new submission manoeuvre the 'Pin-Up Strong'. Phoenix received her title match against Kelly on October 2 at Hell in a Cell, which she won, with Natalya's help, to become a one–time WWE Divas Champion. Phoenix successfully defended her title against Eve Torres, on two different occasions, at Vengeance, on October 23, in which Natalya was banned from ringside after she and Phoenix had attacked Torres and Kelly at backstage, and at Survivor Series, on November 20, during a Divas lumberjack match.
Through November, the Divas of Doom started a winning streak over The Chickbusters (AJ and Kaitlyn), after defeating them in both tag team and singles matches, with Kaitlyn beginning to display villainous traits, due to her being upset at AJ over the defeats. On the December 6 SmackDown tapings, the Divas of Doom defeated The Chickbusters once again. Post match, Kaitlyn solidified her heel turn after joining the Divas of Doom, however the segment was cut from the broadcast and not recognized by WWE.
On January 29, at Royal Rumble, the Divas of Doom competed in an eight-woman tag team match alongside the Bella Twins, and defeated the team of Eve Torres, Kelly Kelly, Alicia Fox, and Tamina. The next night on Raw, Phoenix successfully defended her Divas Championship against Eve. At the Elimination Chamber pay-per-view, Phoenix successfully defended her championship against Tamina, in a point where her association with Phoenix started splitting up, and on the March 22 episode of Superstars, Phoenix teamed with Eve Torres against Natalya and Tamina, in a losing effort, with this effectively ensuring the ending for the team.
Beginning in April, while on NXT Redemption, Natalya became allied with former Hart Dynasty partner Tyson Kidd again, and started feuding with former protégé Kaitlyn when she felt Kaitlyn was paying Kidd too much attention. The pair faced off in both singles and tag team competition throughout mid-2012, including being on opposite sides of a six-Diva tag team match at Money in the Bank, which Natalya's team lost. Their feud ended on August 31, when Natalya lost to Kaitlyn in a singles match on SmackDown. In November, Natalya began an on-screen relationship with The Great Khali. The following month, Natalya saved Hornswoggle from an attack by Rosa Mendes, thus turning face in the process. This led to a feud with Natalya, Khali, and Hornswoggle facing off against Mendes and her allies, Primo and Epico in mixed tag team matches in early 2013. On the March 27 episode of NXT, Natalya lost a Divas Championship match to champion Kaitlyn.
Upon the debut of the Total Divas reality television program in July 2013, Natalya began feuding with fellow co–stars on the show, The Bella Twins. Natalya and Brie Bella went on to trade victories in singles matches on Raw and at SummerSlam. The cast of Total Divas then transitioned into a feud with AJ Lee, the WWE Divas Champion, who ridiculed the cast and the show. This resulted in a four–way match at Night of Champions in September, where AJ successfully retained the title against Natalya, Brie, and Naomi. Simultaneously, Natalya continued appearing alongside long–time ally The Great Khali, and the two began a feud with Fandango and the debúting Summer Rae, which led to a mixed tag team match at the Hell in a Cell pay–per–view, which Natalya and Khali lost. After forcing AJ to submit on the November 1 episode of SmackDown during a tag team match, Natalya unsuccessfully challenged AJ for the Divas Championship on WWE Main Event two weeks later. At Survivor Series, the cast of Total Divas faced off with a team led by AJ and Natalya and Nikki Bella were the sole survivors in the match. In December, Natalya unsuccessfully challenged Paige for the NXT Women's Championship. After pinning AJ again in a tag team match on Raw, Natalya was named number one contender to the WWE Divas Championship, but failed to capture the title at Tables, Ladders and Chairs.
On April 6, 2014, Natalya competed at WrestleMania XXX in the 14–Diva "Vickie Guerrero Invitational match" for the WWE Divas Championship, which was won by the defending champion AJ Lee. In May, Natalya was entered into a tournament to determine the new NXT Women's Champion. She defeated Layla and Sasha Banks en route to the final at NXT TakeOver, in which she lost to Charlotte. Throughout September, Natalya started acting as the on-screen mentor for Rosa Mendes, starting a feud against "The Slayers" (Summer Rae and Layla). They faced off against them during the Main Event and SmackDown shows, losing both tag matches due to miscommunication as a team. Additionally they also faced off against AJ Lee and Paige on the September 8, episode of Raw, once again in a losing effort. On the September 29, episode of Raw, Natalya and Tyson Kidd accompanied Mendes to her match against Layla, in which she was defeated. Following this, her association with Mendes quietly disbanded. On November 23, Natalya took part of Alicia Fox's team at Survivor Series, which was victorious in a clean sweep.
In mid–2014, Natalya entered a storyline with her real–life husband Tyson Kidd, in which their relationship was openly acknowledged on-screen. She regularly accompanied Kidd to the ring, where he often used her as a distraction to win his matches. The storyline would continue following Total Divas footage, in which Kidd transitioned into a disrespectful angle against Natalya, this part of the storyline was done in order to use the marriage problems they both had.
On the January 5, 2015, episode of Raw, after Natalya defeated WWE Divas Champion Nikki Bella in a non–title match, Brie and Nikki would attack Natalya, with Paige making the save. This led to a tag team match at Royal Rumble between the two teams, with The Bella Twins picking up the win. Through February, Natalya and Kidd started a brief feud against Naomi and Jimmy Uso, facing off during an intergender tag team match on the February 16, episode of Raw, which Natalya and Kidd lost. When Kidd allied himself with Cesaro, Natalya began managing the team and was by their side in February, when they won the WWE Tag Team Championships at Fastlane. The following night on Raw, Natalya helped the duo retain the titles against The Usos, turning heel in the process. On the February 26 episode of SmackDown, the villainous Natalya defeated Naomi in a singles match, before the feud ended. On March 28, Natalya inducted Alundra Blayze into the WWE Hall of Fame. On March 29, she accompanied Kidd and Cesaro during the WrestleMania 31 kick-off show, in which they successfully retained the Tag Team Championships.
Natalya lasted the rest of the year competing in various matches, including a number one contender's battle royal for Nikki Bella's Divas Championship, on the April 13 episode of Raw, which was won by Paige. On the April 9 episode of SmackDown, Natalya defeated Alicia Fox. Post-match, she and Fox were attacked by the special guest referee for the match Cameron, which would lead to a triple–threat match the following week, with Cameron coming out victorious. During a dark match on the June 1 episode of Raw, Kidd had suffered a severe neck/spinal injury after receiving Samoa Joe's 'Muscle buster' finishing maneuver. Several weeks later, Kidd stated that he would be out of action for over a year, with Natalya taken off television for the very first time in order to care for Kidd.
After a three-month absence from television, Natalya returned on the September 21, 2015 episode of Raw, as a face, confronting the villainous Paige over her actions during Charlotte's WWE Divas Championship celebration. Later that evening, she was defeated by Naomi in a singles match. After multiple confrontations between the two, Natalya would defeat Paige on the October 5 episode of Raw. Three days later, on SmackDown, Natalya teamed with Charlotte and Becky Lynch and the three defeated Team Bella (Alicia Fox, Brie Bella, and Nikki Bella). On the October 15 episode of SmackDown, while Paige saved Charlotte and Becky from an attack by Team Bella, Natalya, after a backstage altercation with Paige, would be attacked. In the end of October, Natalya started a feud with Team B.A.D. (Naomi, Tamina and Sasha Banks), after the three distracted her during her match with Paige, and attacked her, but Natalya went on to gain revenge over the team by defeating Naomi and Tamina in two singles matches before the feud quietly ended.
In January 2016, Natalya revealed that she had been working through a broken ankle, which was mistaken for a simple sprain and after two months of inactivity, she made her official return during a live event on January 3. A few weeks later, Natalya returned to WWE television, on the January 18 episode of Raw, where she defeated Brie Bella, with her former rival Paige in her corner. Upon her return, Natalya started competing in various singles and tag team matches, ending on both winning and losing sides. On March 12, at Roadblock, Natalya unsuccessfully challenged Charlotte for the Divas Championship.
On the March 22 episode of Main Event, alongside Alicia Fox, she accompanied Paige to her match against Naomi, accompanied by Tamina and Lana. Later in the match, she and Fox were viciously attacked by Summer Rae and a returning Emma, distracting Paige as they aligned themselves with Lana and Team B.A.D. The following week, she along with Brie Bella and Alicia Fox accompanied Paige to her match against Emma on the March 28 episode of Raw, where she was defeated after Lana attacked Paige. Post-match, she along her allies were attacked by Emma, Summer Rae, Lana, Tamina and Naomi, before they were saved by a returning Eva Marie. As a result, Natalya's Total Divas team (also including Brie, Alicia Fox, Eva Marie and Paige) faced the newly dubbed Team B.A.D. & Blonde (Naomi, Tamina, Lana, Emma, and Summer Rae) in a 10-Diva tag team match at WrestleMania 32's pre-show. Natalya's team won after Naomi submitted to Brie Bella. After confronting Charlotte during her championship celebration the following night, she challenged Charlotte to a championship match on the April 11 episode of Raw, in which she was unsuccessful in capturing the WWE Women's Championship. On the April 18 episode of Raw, Natalya confronted Charlotte during an interview and revealed that Shane McMahon had booked them in a rematch for the Women's Championship at Payback and that her uncle Bret Hart will be at her corner. At the event, she was defeated after match referee Charles Robinson, ended the match as Charlotte held her in the Sharpshooter submission hold, Natalya's signature finishing move, even though she had not submitted making reference to the infamous "shoot screwjob" the Montreal Screwjob. After the match, both Natalya and Hart applied their finishing maneuver the "Sharpshooter" on Charlotte and Ric Flair. The following month at the Extreme Rules pay-per-view, she was once again defeated by Charlotte in a submission match in which Ric Flair was banned from ringside, however, she was helped by Dana Brooke while dressed as Flair allowing Charlotte to get the victory.
On June 19 at Money in the Bank, Natalya teamed with Becky Lynch in a losing effort against Charlotte and Dana Brooke. After the match, Natalya attacked Becky, turning into a villainess. Followed by multiple continuous attacks between both women, Natalya defeated Becky in a match at Battleground.
On July 19, Natalya was drafted to SmackDown as part of the 2016 WWE draft. She made her first appearance for the brand on the July 26 episode of SmackDown, losing against Becky Lynch. On the August 9 episode of SmackDown, Natalya competed in a losing effort against Carmella. The following week, Natalya teamed with Alexa Bliss in a losing effort against the team of Carmella and Becky Lynch, after a distraction provided by Eva Marie and Naomi, At SummerSlam, Natalya teamed with Alexa Bliss and the returning Nikki Bella (who replaced the suspended Eva Marie) against Naomi, Lynch, and Carmella in a six-woman tag team match. Nikki Bella pinned Carmella to score the victory for Natalya's team. At Backlash, Natalya competed in a six-pack elimination challenge to determine the inaugural SmackDown Women's Champion and was eliminated by Nikki Bella.
On the October 25 episode of SmackDown, Natalya lost against Nikki Bella in a match to determine the captain of the SmackDown women's team at the Survivor Series pay-per-view. However, after Nikki had been attacked backstage before the match, Natalya replaced Nikki but led her team to defeat. At the TLC pay-per-view, Carmella accused Natalya of having been Nikki's attacker at Survivor Series; Natalya denied this for weeks before attacking Carmella on the December 20 episode of SmackDown and admitting to having attacked Nikki, revealing her pent-up jealousy of Bella's success over the years. Natalya and Nikki were set to compete in a match on the January 10, 2017, episode of SmackDown, but the match never officially started due a brawl between the two, where referees came in to break them up. At the Royal Rumble pay-per-view on January 29, Natalya competed in a six-woman tag team match alongside Alexa Bliss and Mickie James against Nikki, Naomi, and Becky Lynch, where her team was defeated after Naomi pinned Bliss. On February 12 at the Elimination Chamber pay-per-view, Natalya faced Nikki in singles competition, which ended in a double count-out. The feud culminated in a Falls Count Anywhere match on the February 21 episode of SmackDown, in which Natalya was victorious after an interference from Maryse. On June 18 at Money in the Bank, Natalya competed in the inaugural women's Money in the Bank ladder match, which was won by Carmella following an interference by James Ellsworth.
On July 23, Natalya defeated Charlotte Flair, Becky Lynch, Tamina, and Lana in a five-way elimination match at Battleground, earning an opportunity to face Naomi for the SmackDown Women's Championship at SummerSlam on August 20. At the event, Natalya defeated Naomi to capture the SmackDown Women's Championship. With this victory, Natalya became the first woman to hold both the Divas Championship and the SmackDown Women's Championship. On the September 12 episode of SmackDown, Natalya made her first successful title defense in a rematch against Naomi. At Hell in a Cell on October 8, Natalya defended her championship against Charlotte Flair, which resulted into a disqualification loss after she attacked Flair with a chair. On the November 14 episode of SmackDown, she dropped the title to Charlotte, losing by submission, and hereby ending her reign at 86 days. Natalya then competed at Survivor Series along with Becky Lynch, Tamina Snuka, Naomi and Carmella as a part of Team SmackDown against Team Raw in a losing effort. Natalya received her SmackDown Women's Championship rematch at Clash of Champions, but was unsuccessful against Flair in a lumberjack match.
At the Royal Rumble, Natalya participated in the first Women's Royal Rumble Match; she entered at number 18 but was eliminated by Trish Stratus. At Fastlane, Carmellla and Natalya defeated Naomi and Becky Lynch after Carmella pinned Becky.
On the April 16, 2018, episode of Raw, Natalya was once again drafted to Raw and became a fan favorite for the first time since June 2016. In her first match she defeated Mandy Rose, and after the match both Rose and Sonya Deville attacked her, before Ronda Rousey made the save. Shortly after that scene, Natalya was placed in a storyline with Rousey as she was revealed to be her training partner and friend. In June, Natalya competed in the Money in the Bank ladder match for the third time in her career, however, at the event, the match was ultimately won by Alexa Bliss. Throughout the following months, Natalya continued to compete in various singles and tag team matches and also worked as a manager for both Nia Jax and Ronda Rousey in some of their matches against Alexa Bliss to avoid Mickie James' interference.
In October, Natalya joined forces with Sasha Banks and Bayley against The Riott Squad (Sarah Logan, Liv Morgan and Ruby Riott) which led to a six–woman tag team match at the first ever all women's pay–per–view, Evolution, where Natalya, Banks and Bayley were victorious. Shortly after the event, Natalya continued her feud with Ruby Riott after the latter broke the "glasses" of Natalya's recently deceased father. During that time, both women were announced as the final members of Team Raw for the interbrand women's traditional five–on–five tag team elimination match, however, they were eventually removed from the match as they brawled just before Survivor Series started. On the December 3 episode of Raw, in what was supposed to be a tag team match pitting Natalya and Ronda Rousey against Nia Jax and Tamina, The Riott Squad attacked Natalya and put her through a table while Jax and Tamina cornered Rousey to prevent her from helping. This led to a tables match between Ruby Riott and Natalya at the TLC: Tables, Ladders & Chairs event, where Natalya gained revenge and defeated Riott after powerbombing her from the top rope through a table. On the December 24 episode of Raw, after she won an eight woman gauntlet match to become the number one contender a week prior, Natalya faced Rousey for her Raw Women's Championship, however, she was unsuccessful in winning the match and the title.
On January 27, 2019, at the 2019 Royal Rumble, Natalya entered the second women's Royal Rumble match at number 2, lasting 56:01 (surpassing Sasha Banks' previous record set in 2018), and eliminated Liv Morgan and Sarah Logan, before she was eliminated by Nia Jax. At Fastlane, Natalya reunited her team with Beth Phoenix, known as The Divas of Doom, after the two were attacked by Nia Jax and Tamina. The Divas of Doom took part of a fatal four-way tag team match for the WWE Women's Tag Team Championship at WrestleMania 35 on April 7, however, the match was won by the The IIconics (Billie Kay and Peyton Royce). In May, Natalya competed in the Money in the Bank ladder match at the namesake pay–per–view, where she was unsuccessful in winning the match. In June, Natalya and Alexa Bliss were supposed to compete in an late addition match at the Super Showdown pay–per–view in Jeddah, Saudi Arabia, however, the match was rejected by the Saudi Arabian government just before the show started. On 15th July's edition of Raw, Natalya won a fatal four way elimination match to become the #1 contender for Becky Lynch's Raw Women's Championship at SummerSlam. At SummerSlam, Natalya was unsuccessful in winning the Raw Women's title from Lynch in a Submission match. Natalya was defeated by a now-heel Sasha Banks on August 26 edition of Raw. Natalya later began feuding with Lacey Evans, exchanging victories and losses, before defeating her in a last woman standing match. The pair later seemed to gain respect for each other and took on the Kabuki Warriors in a losing effort. Natalya defeated Evans again at Crown Jewel, in which was the first ever women's match to take place in Saudi Arabia. On the WrestleMania 36 kickoff show, she suffered a loss to Liv Morgan.
On the June 15 episode of Raw, Natalya and Liv Morgan lost to The IIconics. Afterward, Natalya teased a heel turn, ripping on Morgan and claiming that she had been given no respect, with Lana venting her frustrations to Natalya afterward. On the June 22 episode of Raw, Natalya turned heel for the first time since 2018, when she solidified her alliance with Lana and defeated Liv Morgan by submission. In August the duo began feuding with the returning Mickie James. As part of the 2020 draft in October, Natalya was drafted to the SmackDown brand. At the beginning of January 2021, Natalya formed an alliance with Tamina while putting the women's tag team division on notice. On the January 30 episode of WWE Backstage, the two allies were forced to face each other in a singles match to determine who would be the number thirty entrant at the Royal Rumble, in which Natalya won, earning her spot. Natalya and Tamina won a tag team turmoil match on night one of WrestleMania 37 for an opportunity to face Nia Jax and Shayna Baszler for the WWE Women's Tag Team Championships. However, on night two, they were unsuccessful. On the April 16 episode of SmackDown, she defeated Shayna in a singles match. On the May 14 episode of SmackDown, she and Tamina would defeat Baszler and Jax to win the WWE Women's Tag Team Championship. After the match, the duo thanked their families and the WWE Universe for cheering them on, turning them face in the process. They would eventually lose the titles to the team of Rhea Ripley and Nikki A.S.H. on the September 20 episode of Raw.
As part of the 2021 Draft, Tamina was drafted to the Raw brand while Natalya remained on the SmackDown brand, ending the team. In October, Natalya entered the Queen's Crown tournament, where she lost to Doudrop in the first round. She would participate in the following January's Royal Rumble, which was unsuccessful. Soon after, she set her eyes on the Women's Tag Team Championships and teamed up with Shayna Baszler over the months, which led to a fatal four-way tag team match at WrestleMania 38, which was won by Sasha Banks and Naomi after Banks pinned Carmella. They would challenge Banks and Naomi after some weeks, leaving them unsuccessful. In June 2022, Natalya would win a six-pack challenge to earn an opportunity against SmackDown Women's Champion Ronda Rousey at Money in the Bank. At the event, Natalya was unsuccessful in defeating Rousey.
On October 28, at a SmackDown taping ahead of Crown Jewel, Natalya suffered a storyline nasal injury during a post-match attack conducted by Shayna Baszler at the instruction of Ronda Rousey, turning her face for the first time since 2020. She returned during the 2023 Royal Rumble match as the eleventh entrant, being eliminated along with Baszler by Damage Control (Bayley, Dakota Kai, and Iyo Sky). On February 5, 2023, Natalya won a fatal four-way match on SmackDown against Baszler, Zelina Vega, and Shotzi to qualify for the women's Elimination Chamber match, where the winner would be given a Raw Women's Championship match against Bianca Belair at WrestleMania 39. On February 18, after starting the match and eliminating Liv Morgan by technical submission with the help of eventual winner Asuka, Natalya was eliminated by Carmella, becoming the third woman in the match to be eliminated overall. On March 25, Natalya teamed with Shotzi to qualify for the women's WrestleMania Showcase fatal four-way tag team match at WrestleMania 39. The match took place on the second night, in which Rousey and Baszler were victorious after Rousey forced Shotzi to tap out with an arm bar. Natalya was drafted to the Raw brand in the 2023 WWE Draft. On the May 8 episode of Raw, Natalya stepped up to SmackDown Women's Champion Rhea Ripley, but Ripley would make her way out of the ring before things got physical. At Night of Champions, Natalya unsuccessfully challenged Ripley for the SmackDown Women's Championship in a squash match that lasted 70 seconds. On the June 8 episode of Raw, Natalya faced Zoey Stark to qualify for the women's Money in the Bank ladder match, but was defeated. On July 3 episode of Raw, Natalya once again unsuccessfully challenged Ripley for the Women's World Championship. On September 6, it was announced that Natalya would once again challenge Ripley for the Women's World Championship at Superstar Spectacle; Natalya was defeated at the event. On the September 18 episode of Raw, Natalya unsuccessfully challenged Becky Lynch for the NXT Women's Championship. Over the following weeks, Natalya would form a tag team with Tegan Nox. On the November 27 episode of Raw, the duo unsuccessfully challenged Chelsea Green and Piper Niven for the WWE Women's Tag Team Championships.
On January 27, 2024, at the 2024 Royal Rumble, Natalya entered the women's Royal Rumble match at number one and lasted 20:57. During the match, she attempted to eliminate her tag team partner Tegan Nox before being eliminated by Nox herself. On the April 9 episode of NXT, Natalya unsuccessfully challenged Roxanne Perez for the NXT Women's Championship, after interference from Lola Vice. During week two of NXT Spring Breakin' on April 30, Natalya was defeated by Vice in an NXT Underground match. Natalya next participated in the 2024 Queen of the Ring tournament, where she was defeated by Iyo Sky in the first round. On September 9 episode of Raw, Natalya made her comeback after a three-months hiatus to team up with Lyra Valkyria and Zelina Vega, defeating Pure Fusion Collective (Shayna Baszler, Sonya Deville and Zoey Stark).