"The Supremes Produced and Arranged by Jimmy Webb" marked a departure from the Motown Sound that the Supremes had relied upon over the past decade, and moved the group out of its pop/R&B genre and into a rock/pop style masterminded by Webb. The result was an album that had a different sound to that which the public, and the Supremes themselves, were accustomed. On many of the tracks, Webb overdubbed additional background vocals by The Blossoms, in addition to the voices of Wilson and Laurence. Terrell sings lead on all of the tracks on the LP, except "I Keep It Hid", which features Wilson on lead vocals. Terrell duetted with Webb on "Once in the Morning".