She & Him, the duo she formed with M Ward, will release their next album later this year on the Sony label, reported Billboard.
The pair has released four albums on independent label Merge Records and has sold just over one million records since 2008.
The duo's bestseller was 2011 holiday album A Very She & Him Christmas.
She & Him aren't the only act to leave Merge - Spoon and Arcade Fire have reportedly departed the label after enjoying initial success there.
M Ward is still signed to Merge as a solo artist.