In the summer of 1959, a talent scout from Warner Bros. saw the heavy-set Buono play "Falstaff" at the Globe and took him to Hollywood for a screen test. Buono made his first network TV appearance playing the bearded poet Bongo Benny in an episode of "77 Sunset Strip." Over the next few years, he played menacing heavies in series on TV and appeared on "The Untouchables." After appearing in a few uncredited film roles, he was cast by director Robert Aldrich in the psychological horror movie "What Ever Happened to Baby Jane?" (1962). The film starred Bette Davis and Joan Crawford, and Buono played the hapless musical accompanist Edwin Flagg, a performance for which he was nominated for the Academy Award for Best Supporting Actor and the Golden Globe Award for Best Supporting Actor – Motion Picture.