Harris released her solo debut, Gliding Bird, in 1969 on fledgling Jubilee Records.

In 1973, Harris was invited to join Gram Parsons' band The Fallen Angels on the recommendation of Chris Hillman, then playing with Parsons' former band, The Flying Burrito Brothers. Harris collaborated with Parsons on his final album, Greivous Angel, in the months before his death from a drug overdose.

Harris released her major label solo debut, Pieces of the Sky, in 1975 on Reprise Records. Hoping to reach a bigger audience, she formed The Hot Band (so named because a record executive had advised her to "get a hot band"), and released her follow-up, Elite Hotel, in 1975. It won a Grammy in 1975 for Best Country Vocal Performance, Female.

Harris continued releasing commercially and critically successful albums throughout the remainder of the 1970s, 1980s and 1990s, and collaborated with artists including Dolly Parton, T-Bone Burnett, Willie Nelson, Linda Ronstadt, Vince Gill and the Nitty Gritty Dirt Band. She recently appeared on Neil Young's acclaimed Prairie Wind album and in the Jonathan Demme-directed concert film Neil Young: Heart of Gold.