Terrell's career began as a teenager, first recording for Scepter/Wand Records, before spending nearly 9 months as a member of James Brown's Revue, recording for Brown's Try Me label. After a period attending college, Terrell recorded briefly for Checker Records, before signing with Motown in 1965. With Gaye, Terrell scored seven Top 40 singles on the "Billboard" Hot 100, including "Ain't No Mountain High Enough" which was inducted into the Grammy Hall of Fame in 1999, "Ain't Nothing Like the Real Thing" and "You're All I Need to Get By". Terrell's career was interrupted when she collapsed into Gaye's arms as the two performed at a concert at Hampden–Sydney College on October 14, 1967, with Terrell later being diagnosed with a brain tumor. She had eight unsuccessful surgeries before succumbing to the illness on March 16, 1970 at the age of 24.