In 1964, Albano wrestled for the World Wide Wrestling Federation as a singles competitor.
He returned in 1967 alongside Tony Altomare. In July, they won the WWWF United States Tag Team Championship from Arnold Skaaland and Spiros Arion. Albano and Altomare only held the championship for two weeks. By 1969, the Sicilians disbanded and went their separate ways; Albano went on as a singles competitor.
In 1970, Crusher Verdu debuted in the WWWF. His in-ring capabilities were hampered by a limited command of English, and Albano was assigned to be his mouthpiece. Albano emphasized Verdu's physique and insisted that he had never been taken off his feet during a match. Verdu faced Bruno Sammartino in June 1970. After losing that match, Verdu cycled out of the WWWF rotation, but Albano remained as the top heel manager for the next 15 years.
Thus began his transition into the brash, bombastic manager "Captain" Lou Albano. With a quick wit and a grating personality, Albano delivered memorable promos and earned the scorn of the wrestling audience as he attempted to dethrone World Wide Wrestling Federation (WWWF) superstar and Heavyweight Champion Bruno Sammartino. Growing out his hair and beard, and packing on extra pounds, Albano gave the image of a wild man. He developed a later trademark, applying rubber bands to his beard. He also often wore a rubber band hanging from a safety pin pushed through his cheek.
In January 1971, Albano was the manager when Ivan Koloff ended Sammartino's seven-year reign as champion. Koloff's title reign was a transitional one, lasting just three weeks. Koloff had a typical heel run against Sammartino in 1969, but Albano spent months claiming that his previous manager had trained him incorrectly, and that Koloff would beat Sammartino under Albano's expert tutelage. The shock of Koloff's victory was such that the crowd fell totally silent, and Sammartino momentarily feared that he'd lost his hearing.
Albano then resumed his role as the mastermind trying to lead his latest bad guy protege to the gold. For the remainder of the 1970's and into the mid-1980's, Albano's cadre of loyal henchmen were unable to re-secure the heavyweight championship, held by either Sammartino, Pedro Morales, Bob Backlund or Hulk Hogan. However, Albano guided singles wrestlers Don Muraco and Greg Valentine to the Intercontinental Heavyweight Championship. Furthermore, Albano guided fifteen teams to the WWF World Tag Team Championships, including The Valiant Brothers, The Wild Samoans, The Yukon Lumberjacks, The Blackjacks, The Moondogs, The Masked Executioners, and after becoming a face, the U.S. Express and the British Bulldogs. It was during his stewardship of the Valiant Brothers that Albano picked up his "Captain" nickname, as the act was promoted as "Captain Lou and the Valiants too." By the end of his career, Albano had managed over 50 different wrestlers who won two dozen championships.
Albano could also help elevate wrestlers by splitting from them. In 1982, despite being managed by the villainous Albano, Jimmy Snuka was unexpectedly becoming a fan favorite due to his high-flying ring style. An interview segment revealed that Snuka had no legal contract with Albano, and thus was able to leave his manager. Shortly thereafter, a bloody beatdown by Albano, Freddie Blassie and Ray Stevens, helped transform Snuka into a sympathetic figure, and triggered the most successful period of his career. Albano had previously helped turn the villainous Intercontinental Champion Pat Patterson into a fan favorite, by "purchasing" Patterson's contract against his will. He also managed the U.S. Express at WrestleMania.
In 1984, Albano began feuding with celebrity Cyndi Lauper. Albano and Lauper agreed to compete by proxy, each choosing a female wrestler to contend. Lauper chose Wendi Richter, while Albano chose The Fabulous Moolah. The match, scheduled for July 23, 1984, was dubbed The Brawl to End it All, and was broadcast live on MTV. During the match, Lauper interfered on Richter's behalf by hitting Moolah in the head with her purse, dubbed "The Loaded Purse of Doom". At the conclusion of the match, Richter had defeated Moolah for the WWF Women's Championship, which the WWF had promoted Moolah as having held for the previous 28 years.
In 1984, Albano decided it was time, after 32 years as a heel, to turn face. He therefore arranged for Lauper to receive an in-ring award for her contributions to wrestling, for which he also came out and congratulated her. In the course of the ceremony, Roddy Piper and "Cowboy" Bob Orton came into the ring to sarcastically praise Albano before breaking Lauper's award, a gold record plaque, over his head. Lauper and her boyfriend-manager David Wolff were also attacked by Piper and Orton. The melee was broken up by Hulk Hogan, but the altercation allowed Albano to now wrestle and manage as a crowd favorite.
His last two (heel) singles protégés, Greg Valentine and Ken Patera, were paired with Jimmy Hart and Bobby Heenan, respectively, after Albano's face turn. Although he continued his overblown, rambling interviews, Albano was now leading fan favorites such as The U.S. Express, George Steele, The British Bulldogs, Hulk Hogan and André the Giant into battle. The U.S. Express and British Bulldogs became the first tag teams to win the WWF Tag Team Championships with Albano as a "face" manager.
Albano left the WWF in late 1986 with one final match on an episode of Wrestling Challenge that aired on November 16, 1986, teaming with The British Bulldogs to defeat The Dream Team and "Luscious" Johnny Valiant. Albano would then make a one-time appearance on Piper's Pit on an episode of Superstars of Wrestling in February 1987 to ask André the Giant to reconsider his recent alignment with Bobby Heenan.
Albano returned to the WWF in 1994 to manage the newly face-turned Headshrinkers, helping lead them to the WWF Tag Team Championship. He left in early 1995, making sporadic appearances as a guest from then-on, but never as a manager.
In 1996, Albano was inducted into the WWF Hall of Fame.
On October 14, 2009, Albano passed away.