Tammi Terrell began recording for Scepter/Wand Records at the age of 15, before touring with the James Brown Revue for a year. Terrell's talents won her a contract with Motown Records in Detroit, Michigan later that year, at which time she changed her stage name to Tammi Terrell (contrary to popular belief, Terrell did not marry boxer Ernie Terrell, brother of future Supremes lead singer Jean Terrell).

In the mid-1960s, Terrell released a series of minor R&B chart hits, among them "I Can't Believe You Love Me", "Come On and See Me", and a cover of The Isley Brothers' "This Old Heart of Mine". In 1967, she was selected to replace Kim Weston as Marvin Gaye's recording partner. This teaming produced Gaye's most successful duets, and the pair issued a stream of hit singles between 1967 and 1969. "Ain't No Mountain High Enough" and "You're All I Need To Get By" epitomized their style, as Gaye and Terrell wove around each other's voices, creating an aura of romance and eroticism that led to persistent rumors that they were lovers. Most of the Gaye/Terrell duets were crafted by two songwriting/production teams: Ashford & Simpson and Harvey Fuqua & Johnny Bristol

While on tour with Gaye in Virginia during the summer of 1967, Terrell fainted onstage. She was diagnosed as suffering from a brain tumor, and despite a series of major operations over the next three years, her health steadily weakened. By 1969, Terrell was too weak to perform in public or in the studio, and the duo's co-producer, Valerie Simpson, subbed for Terrell on many of the duo's final recordings. Ironically, one of these tracks, "The Onion Song", proved to be the most successful of the Gaye/Terrell singles in the UK.

Tammi Terrell died on March 16, 1970, her burial service attracting thousands of mourners, including many of her Motown colleagues.

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