Harmony is the follow-up to Never Shout Never's critically heralded debut What Is Love?, which bowed at No. 24 on the Billboard Top 200 album chart, No. 2 on both the Alternative and Rock charts, No. 6 on the Digital Album chart, and No. 11 on the Internet album chart upon its release in January.

The album was produced by veteran producer Butch Vig, who is best-known for his work with Green Day, Nirvana, and Smashing Pumpkins.