Carter recorded for Sam Cooke's SAR record label in the early 1960s. He had his first hit in 1962 at the age of nineteen with "When a Boy Falls in Love", which was co-written by Cooke.

By the time he reached his commercial peak with Imperial Records in the middle of the decade, he was specializing in pop ballads. His biggest success was the Top 10 Billboard Hot 100 hit, "Hold Me, Thrill Me, Kiss Me," in 1965. It sold over one million copies, and was awarded a gold disc. He had a couple of other Top 40 entries over the next year, "Band of Gold" and "All of a Sudden My Heart Sings", as well as a few other easy listening sellers.

Carter appeared on the DVD of the PBS special, Doo Wop 51, recorded in 2001 performing his hit.

Carter later acted on television programmes such as Quincy, M.E., Sanford and Son, Marcus Welby, M.D. and Magnum, P.I..