In 1960, Maharis appeared as Buz Murdock in the TV series Route 66, which co-starred Martin Milner. Maharis was 32 at the time the series started, although the character he was playing was only 23. He received an Emmy nomination in 1962 for his continuing performance as Buz.

Maharis released albums and singles through Epic Records earlier in his career. His only top-40 pop hit was his version of the standard “Teach Me Tonight”, which hit number 25 in June 1962, although several other singles charted below the top 40. Later, he performed in nightclubs and pursued a secondary career as an impressionist painter. As of 2008, Maharis was still painting, splitting his time between New York and Beverly Hills.

Maharis said he left Route 66 for health reasons, due to long hours and grueling conditions while shooting on location. “I have to protect my future”, Maharis said in a 1963 interview. “If I keep going at the present pace, I’m a fool. Even if you have $4,000,000 in the bank, you can’t buy another liver.”

Returning to series television in 1970, Maharis starred as criminologist Jonathan Croft in The Most Deadly Game. The series lasted 12 episodes, ending in January 1971.

Throughout the 1970s and 1980s, Maharis guest-starred in many television series, including Mission: Impossible, Fantasy Island, Kojak, McMillan & Wife, Barnaby Jones, Police Story, Switch, Cannon, Night Gallery, and The Bionic Woman, as well as Murder, She Wrote in 1990.