After moving to Los Angeles and becoming a regular performer at the influential Hotel Cafe venue, Brothers first gained national attention with his song "Blue Eyes" on the Platinum-selling, Grammy-winning "Garden State" soundtrack.

Brothers plays regularly as part of the musical community at the Hotel Café in Los Angeles,[7] and he has since toured across America and Canada with such acts as Greg Laswell, Sara Bareilles, Liz Phair, KT Tunstall, Aqualung, Ben Lee, Matt Nathanson, Imogen Heap, and The Fray.

In 2007, Cary Brothers signed a record deal with indie label Bluhammock Music for the release of his first full-length album, Who You Are, on May 29, 2007, which made the Billboard Heatseekers Chart.

[9] Produced by Chad Fischer (Alexi Murdoch) and mixed by Greg Collins (Grammy Winner – U2), the record features guest musicians Matt Hales from Aqualung and Priscilla Ahn.

He helped close Friday night at Bonnaroo in the summer of 2008 by making a guest appearance with Tiësto and repeated this musical pairing a few months later at the O2 arena in London.

[12] In addition, that year he had an original track called "Here on Earth" on the Tiësto record Kaleidescope alongside Sigur Rós, Tegan and Sara, Kele Okereke, Priscilla Ahn and Emily Haines.

[20] In spring 2023, Brothers appeared in the film A Good Person, performing his single "Stardust" for the main character Allison (played by Academy Award-nominee Florence Pugh).