Although founding member Florence Ballard is pictured on all album artwork and sings on all the tracks, by the time the set was released, she had been fired from the group and replaced by Cindy Birdsong.

[5] Greatest Hits includes fifteen Supremes singles, 10 of which went to number-one, among them were "Where Did Our Love Go", "Stop!

The packaging for the set includes liner notes by actress Carol Channing (which were originally written for the unreleased album The Supremes and the Motown Sound: From Broadway to Hollywood) and paintings by Robert Taylor, including collectable 12 inch by 12 inch pin-up portraits of Diana Ross, Florence Ballard, and Mary Wilson.

Greatest Hits was their second number-one album on the Billboard 200 and their fifth on the Hot R&B LP's charts in the United States.

Although not nominally credited because of their increasingly estranged relationship with Motown, all of the songs included were produced by the songwriting/production team of Holland–Dozier–Holland.