He joined Duran Duran in 1980 after his ex-girlfriend Fiona Kemp (a bar maid at the Rum Runner club where Duran got their start) introduced him to the band. The band's first album, Duran Duran, was released in 1981, and they quickly shot to fame as part of the New Romantic movement. Three more albums followed in quick succession: Rio (1982), Seven and the Ragged Tiger (1983) and Arena (1984). He appeared as one of the vocalists on the 1984 Band Aid charity single, Do They Know It's Christmas.
While Duran Duran was on hiatus in 1985, Le Bon formed the band Arcadia with fellow Duran Duran members Nick Rhodes and Roger Taylor, releasing only one album So Red the Rose (1986).
Duran Duran's success began to wane in the late 1980s, although they had a resurgence in popularity in 1993 with The Wedding Album. The band will reportedly release a new album in 2004.
Simon Le Bon married model Yasmin Le Bon (nee Parvaneh) on December 27, 1985 and they have three daughters, Amber (born 1989), Saffron (1990) and Tallulah (1994).