Buono made a guest appearance as Hannibal Day in the Get Smart episode "Moonlighting Becomes You", originally airing January 2, 1970, and appeared three times as Dr. Blaine in the sitcom Harrigan and Son, starring Pat O'Brien and Roger Perry as a father-and-son team of lawyers. He appeared in a segment of Night Gallery titled "Satisfaction Guaranteed". He also appeared in an episode of Hawaii Five-O, "The $100,000 Nickel", in which he played thief Eric Damien. It first aired on December 11, 1973. He made two memorable appearances on The Odd Couple, once in the episode "The Exorcists" and again in "The Rent Strike", where he portrayed Mr. Lovelace. In 1976, he appeared in comedy The Practice, portraying Bernard on the episode "Jules and the Bum". He also made nine appearances on the 1977 series Man from Atlantis, appearing all nine times as Mr. Schubert, the enemy of the main character.