Laure is also a film Actress, appearing in a number of Canadian-produced films, including the controversial 1974 release by Dušan Makavejev Sweet Movie, which was notable for both its sexual explicitness and scatology. Laure and Furey were frequent co-stars in the films of Gilles Carle, most notably, L'Ange et la femme (1977) and Fantastica (1980).

Throughout most of her career, Carole Laure primarily collaborated with Anglophone singer, Songwriter, Producer, and Director Lewis Furey, whom she met in 1977 and who later became her husband.

Laure debuted as a singer on the album Alibis in 1978.

In 1989, she devoted an acoustic-oriented bilingual album, Western Shadows, to country and western standards. The album featured cover versions of Tammy Wynette's "Stand By Your Man", Phil Spector's "To Know Him is to Love Him", Rosanne Cash's "Seven Year Ache", and Leonard Cohen's "Coming Back to You". The video for "Danse avant de tomber" (a cover of Boris Bergman's French adaptation of Doc Pomus' "Save the Last Dance For Me") featured Dancer Louise Lecavalier of the internationally famous Québéc contemporary dance troupe La La La Human Steps.

For her 1991 album She Says Move On, she recorded a cover version of Jimi Hendrix's "Purple Haze".

She switched from acoustic to electronic music on her 1997 French-language album Sentiments Naturels. The album featured club-oriented genres such as techno, house, and trip hop, and collaborators included Dimitri from Paris, Mirwais, Shazz, DJ Cam, and Todd Terry. Laure was also named in the songwriting credits.

Laure was appointed an Officer of the Order of Canada in 2013, "For her international career as an Actress, singer, Director and Dancer."