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Before signing to a big record label, Carlile, Tim and Phil Hanseroth, performed in the following local Seattle establishments: The Crocodile, Tractor Tavern, various restaurants and a Sunday night gig at Paragon Grill in Queen Anne. Carlile sold their self-released recordings during their local performances. Slowly doors started opening for Carlile, after Dave Matthews heard them perform at the 2003 Sasquatch music festival and after recording background vocals on Melissa Etheridge's "Lucky" album.
Columbia Records signed Carlile in late 2004 on the strength of songs she had been recording periodically at home. Released in 2005, Brandi Carlile showcased those early songs along with several newly recorded tracks. Shortly after the release of Brandi Carlile, she left her home in Seattle and set out with the Hanseroth brothers, with whom she'd worked on her earliest recordings and independent regional tours. The tightly knit trio, which forms the core of her band today, spent the better part of two years on the road honing the songs that would later become part of her album The Story.
In 2005, she was featured on Rolling Stone's "10 Artists to Watch in 2005" list.By the end of 2006, Carlile had embarked on several headlining tours and supported a variety of artists including Ray LaMontagne, Johnny Lang, Hanson, Indigo Girls, The Fray, Chris Isaak, Tori Amos, and Shawn Colvin.
Her second album, The Story, was released in April 2007. It was produced by T Bone Burnett and includes a collaboration with the Indigo Girls on "Cannonball." The album was recorded in an eleven-day-long session with Carlile, the twins (Tim and Phil Hanseroth), cellist Josh Neumann and drummer Matt Chamberlain to capture the sound of Carlile's live performances. The crack in Carlile's vocals during the title track, "The Story", came out by accident and was a direct result of the way the album was recorded. Carlile herself describes the vocals as "technically wrong but emotionally right."
Carlile was exposed to a wider audience when ABC's Grey's Anatomy showcased three of her songs: "Tragedy," "What Can I Say," and "Throw It All Away". In April 2007, Grey's Anatomy debuted a version of the video for the single The Story interspersed with footage from the show. On May 3, 2007, a special two-hour episode of "Grey's Anatomy" featured Carlile's song "Turpentine" during footage of the "Grey's Anatomy" spin-off, Private Practice.
In November 2007 Carlile visited the UK for her first ever UK gig at the Borderline in London. In February 2008, Carlile performed as special guest to Newton Faulkner on five of his UK tour dates. In March and April 2008 Carlile toured through Australia with Maroon 5 and OneRepublic. In April 2008 she played four dates in the UK and was a guest performer on the BBC2 show, Later... with Jools Holland. Carlile's album The Story was released in the UK on April 21, with lead single "Turpentine" released on April 14.

Charity activities

Carlile worked with Reverb, a non-profit environmental organization, for her 2007 fall tour. She also performed with Ben Taylor in the Eden Presents…Alive In The World concert series for the benefit of Eden Florida, an organization that assists autistic children and adults