Twomey and the Avetts decided to document their side project in 2000, and "the Back Door Project" was renamed the Avett Brothers with the release of a self-titled album that same year. Nemo broke up before 2000 came to a close, and Seth and Scott decided to make the Avett Brothers their new priority. They amicably parted ways with Twomey and added upright bassist and vocalist Bob Crawford to the combo. After a few months of playing live shows, the new trio recorded its second album, 2002's Country Was. The Avett Brothers hit the road upon the album's release that summer, and used the opportunity to break in material for their next studio project, A Carolina Jubilee, which was released in 2003. (A live disc, Live at the Double Door Inn, was sandwiched between the two studio sets.)
Over the next several years, the Avett Brothers maintained a busy and prolific schedule. They released a lengthy and ambitious studio album, Mignonette, in 2004, another live disc in 2005, and both a full-length album (Four Thieves Gone: The Robinsville Sessions) and an EP (The Gleam) in 2006, all recorded during breaks in the group's heavy touring calendar. As if this weren't enough to keep the three men occupied, Crawford also recorded and performed with his side project New Jersey Transient, Seth Avett released albums under the moniker Darling, and Seth and Scott occasionally played shows with their electric band Oh What a Nightmare. In 2007, the Avett Brothers reached a new level of popularity with Emotionalism, their first album to make a dent on the Billboard charts. Rick Rubin took notice and signed the band to American Recordings, his own division of Sony BMG/Columbia, during the summer of 2008. The Gleam II, issued just several months later, was the Avett Brothers' last release on the Ramseur label, while 2009's I and Love and You served as their major-label debut.