Buono was cast to play villains of various ethnic origins on many television programs between 1960 and 1970. He was cast twice in 1960 in the western series "The Rebel," starring Nick Adams, in the episodes "Blind Marriage" and "The Earl of Durango". In 1962, he played Melanthos Moon in an episode of "The Untouchables," titled "Mr. Moon", where he played a San Francisco art and antique dealer who hijacked a supply of the paper used for printing United States currency. In a 1963 episode of the same series, titled "The Gang War", he played Pamise Surigao, a liquor smuggler competing with the Chicago mob.