Gardot started music lessons at the age of nine and began playing piano in Philadelphia bars at the age of sixteen on Fridays and Saturdays for four hours a night. She insisted on only playing music she liked, ranging from standards from The Mamas & the Papas to Duke Ellington and modern groups such as Radiohead.
During her time in hospital she learned how to play the guitar and began writing songs, which were made available as downloads in iTunes and released in Some Lessons: The Bedroom Sessions in 2005. She began to play these songs at venues in Philadelphia and was spotted by the radio station WXPN, operated by the University of Pennsylvania in Philadelphia, which helped to launch Norah Jones. As well as playing her songs, WXPN encouraged her to assemble a demo, which was quickly picked up by Universal Records.
Released in 2006 and then re-released by Verve Records in 2008, her first full-length album was entitled Worrisome Heart. After meeting her in New York City in 2008, producer Larry Klein began working with Gardot and they released her second album, My One and Only Thrill, on April 28, 2009. From this album, the song "Who Will Comfort Me?" became a top 10 hit at Smooth Jazz radio. Also in 2009, Gardot released a live EP, Live from SoHo. Gardot is a recipient of the 2007 VSA International Young Soloists Award.