Brill met his wife, Actress Mitzi McCall, when they both appeared at the Jerry Lewis Comedy Workshop at Paramount Studios in 1959. The couple have one daughter, Jennifer Brill.
Brill and McCall performed Sketch comedy on The Ed Sullivan Show on the same episode as the Beatles first appearance, February 9, 1964. They were interviewed in 2005 for the "Big Break" episode of PRI radio program This American Life regarding their Beatles-Sullivan experience, including a dressing room encounter with John Lennon.
Brill's first motion picture was The Beast of Budapest. He appeared in Blackbeard's Ghost and The Amazing Dobermans. He played Arne Darvin in the Star Trek episode "The Trouble with Tribbles" (1967) and Star Trek: Deep Space Nine episode "Trials and Tribble-ations" (1996). He and his wife, Mitzi McCall played Capt. Harry Lipschitz and Mrs. Lipschitz, on the long-running series Silk Stalkings.
In 1968-69, Brill and McCall appeared on Rowan and Martin's Laugh-In, but only as the violently bickering couple in "The Fun Couple" sketches. Brill was a frequent panelist on the 1970s revival of Match Game and, along with McCall, the celebrity-couples game show Tattletales.
