The Maroon 5 frontman and Voice coach will make his acting debut in FX drama American Horror Story, and is now moving into film work.
Deadline reports that Levine will join Keira Knightley, Mark Ruffalo and Hailee Steinfeld, who have already been cast in the John Carney-directed film.
Carney last helmed the intimate 2006 film Once, which has since been turned into a Tony award-winning Broadway show.
Levine will play Knightley's boyfriend, and the film's plot sees them both moving to New York to pursue careers in music. After he dumps her for a solo contract, she is discovered in a local bar by Ruffalo's record producer.
He recently expressed interest in appearing on Glee, which shares its creator and executive producer Ryan Murphy with American Horror Story.
Watch a trailer for Once below: