Faithfull was first discovered at a London party by Rolling Stones manager Andrew Loog Oldham, who introduced her to Jagger and Richards. Faithfull's rendition of "As Tears Go By"

Faithfull played herself in Jean-Luc Godard’s 1966 movie “Made in U.S.A.,” starring Anna Karina, and made her debut onstage co-starring in Chekhov’s “Three Sisters” with Glenda Jackson. She starred alongside Alain Delon in the 1968 film “The Girl on a Motorcycle,” and worked with other heavy hitters including Orson Welles and Oliver Reed.

She and Jagger began dating in 1966 and became one of the most glamorous and notorious couples of 1960s “Swinging London.”