Smith released her debut album, Elemental, under the auspices of CBC Variety Recordings in 1989. It was recorded at CBC Halifax. Alas, unbeknownst to Smith or CBC, at about the same time, Loreena McKennitt released an album with the same title, so Smith's debut release was changed to Laura Smith when she leased back the masters from CBC. Her second album, B'tween the Earth and My Soul (1994) brought her national acclaim and earned her two East Coast Music Awards (Female Artist, Album of the Year) and two Juno nominations for Best New Solo Artist and Best Roots and Traditional Album. The next year, 1997, she was awarded a Gemini Award for Best Performance in a Performing Arts Program or Series.
She continued to work through the 2000s, including two seasons on stage in Prince Edward Island in the role of Marilla in the musical Anne & Gilbert at the Victoria Playhouse in Victoria-by-the-Sea and the Jubilee Theatre in Summerside respectively. However, through the decade she suffered three debilitating accidents which resulted in chronic pain. This led to the use of increasingly stronger prescription drugs which eventually led to dependence. She attempted to obtain a Music Therapy degree from Acadia University, but gave up her studies to concentrate on healing. She disappeared from the music scene for a time, but by 2010 she was performing again, having overcome her dependency through the adoption of non-narcotic pain treatment therapies. Her story was featured in a radio documentary which aired on CBC Radio One's morning program The Current on February 3, 2010. In 2010 and 2011 she performed several shows across Canada, touring with Ryan MacGrath.
In 2012 Cathie Ryan recorded a version of Smith's "I'm a Beauty" on her album Through Wind and Rain.
Smith completed her first recording in sixteen years, Everything Is Moving, in January 2013. It was released by Borealis Records on April 10, 2013.