It includes hit singles by the group on both the Epic and Imperial labels over a time span of 1965 to 1971.

Since the group did not figure prominently on the American singles chart until late 1965, this compilation misses songs that had been big hits for the Hollies in the United Kingdom such as "Stay," "Here I Go Again," and "I'm Alive."

Nine of the tracks feature founding member Graham Nash during his tenure in the band through 1968.

Greatest Hits was reissued on compact disc by Legacy Records on March 26, 2002.

The remastered version added a bonus track, "The Air That I Breathe" from 1974, which was the Hollies' last top ten song in the U.S.