The first disc features the original Pop album, while the second disc collects the Burning Skies and Tones on TailEPs, along with the "Lions", "Christian Says", "There's Only One" and "Performance" singles. The order of songs "When You're Smiling" and "You, the Night and the Music" was reversed on this compilation. Included as a bonus is a live performance of Elvis Presley's "Heartbreak Hotel" (the only officially released live recording), followed by a radio interview with Daniel Ash.
A handful of alternate mixes were not released as part of this collection: the radio edits of "GO!" and "Burning Skies", as well as an extended mix of "Twist", were released on the promo disc Something!
"Copper" was originally designated as playable at either 45 or 331⁄3RPM, as it was originally released on vinyl; the 45 RPM version of the song is included in this set.
Writing a review for Allmusic, critic Ned Raggett said that the need for a complete compilation of Tones on Tail work "was long overdue". Describing the group's underground hit "Go!", he said: "It remains a wonderful, atypical dancefloor smash, with Ash's loopy 'ya-ya' chorus, Haskins' nutty percussion patterns, Campling's great fuzz bassline, and more all coming together in weird and fun ways."  Referring to the "Twist"/"Go!" single, James Muretich of The Calgary Herald said: "The guitar lines are dark and playful, a strange but effective combination."  Richard Williams of The Michigan Daily said: "Pop attends to a myriad of textures. Most of them poking sinister fun at the conventions of pop music."  Ned Raggett described Pop as "an impressive, wide-ranging effort collaging a range of influences into an inspired, often unpredictable experience."