Langhorne worked with many of the major performers in the folk revival of the 1950s and 1960s, including The Clancy Brothers & Tommy Makem, Joan Baez, Richie Havens, Carolyn Hester, Judy Collins, Peter LaFarge, Gordon Lightfoot, Hugh Masekela, Odetta, Babatunde Olatunji, Peter, Paul and Mary, Richard and Mimi Fariña, Tom Rush, Steve Gillette, and Buffy Sainte-Marie.

[2] The title character of Bob Dylan's song "Mr. Tambourine Man" was probably inspired by Langhorne, who used to play a large Turkish frame drum in performances and recordings.

[3][4] The drum, which Langhorne purchased in a music store in Greenwich Village, had small bells attached around its interior, giving it a jingling sound much like a tambourine.

[3][6] He also played the guitar for Dylan's television performances of "It's Alright Ma (I'm Only Bleeding)" and "It's All Over Now, Baby Blue" on The Les Crane Show in February 1965, a month after the Bringing It All Back Home sessions.

He also provided the scores for Fonda's 1973 science fiction film Idaho Transfer and his 1976 vigilante movie Fighting Mad (directed by Jonathan Demme).