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During recording sessions, Gaye would recall later that he did not know how gifted Terrell was until they began singing together. For sessions of their first recording, the Ashford & Simpson composition, "Ain't No Mountain High Enough", both Gaye and Terrell recorded separate versions. At the end of the year, the duo scored another top ten single with "If I Could Build My Whole World Around You", which peaked at No. Throughout that year, Gaye and Terrell began performing together and Terrell became a vocal and performance inspiration for the shy and laid-back Gaye, who hated live performing.Motown remixed the vocals and edited out the background vocals, giving just Gaye and Terrell vocal dominance. Their follow-up, "Your Precious Love", became an even bigger hit, reaching No. The duo also performed together on television shows to their hits.However, on October 14, 1967, while performing with Gaye at Hampden–Sydney College, After recovering from her first surgery, Terrell returned to Hitsville studios in Detroit and recorded "You're All I Need to Get By".Both that song and "Ain't Nothing Like the Real Thing", reached No. Despite Terrell's optimism, her tumor worsened requiring more surgeries.Following this relative failure, Terrell announced a semi-retirement from the music business and enrolled in the University of Pennsylvania where she majored in pre-med, staying at the school for two years.In the middle of this, Terrell was asked by Jerry Butler to sing with him in a series of shows in nightclubs.
In early 1967, Motown hired Terrell to sing duets with Marvin Gaye, who had achieved duet success with Mary Wells and Kim Weston as well as having recorded duets with Oma Heard. The song's B-side, the Marvin Gaye composition "If This World Were Mine", became a modest hit on both charts (No. All four songs were included on Gaye and Terrell's first duet album, United, released in the late summer of 1967.
Terrell agreed and signed with the label on April 29, her 20th birthday.