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Laurent began acting at age sixteen, cast by Gérard Depardieu in a small role in the romantic drama The Bridge (1999). She gained wider recognition for supporting work in several French films, including the comedy Dikkenek (2006), for which she won Étoiles d'Or for Best Female Newcomer. Her breakthrough role came in the 2006 drama film Don't Worry, I'm Fine, for which she won the César Award for Most Promising Actress and the Prix Romy Schneider. Laurent made her Hollywood debut in 2009 with the role of Shosanna Dreyfus in Quentin Tarantino's blockbuster war film Inglourious Basterds. Her performance won the Online Film Critics Society and the Austin Film Critics Association Best Actress Awards.

While she has worked mainly in independent films, including Paris (2008) and Enemy (2013), Laurent also appeared in commercially successful international films, including the comedy-drama Beginners (2011) and the caper film Now You See Me (2013), the former earning her a nomination at the San Diego Film Critics Society Award for Best Supporting Actress. Her other notable works include the art-house drama The Round Up (2010), the comedy-drama The Day I Saw Your Heart (2011), and the mystery thriller Night Train to Lisbon (2013). She is also known for voicing Mary Katherine and Disgust in the French dubs of Epic (2013) and Inside Out (2015). Additionally, she starred in Chris Weitz's 2018 drama Operation Finale, telling the story of the capture of Nazi Adolf Eichmann.

In addition to her film career, Laurent has appeared in stage productions in France. She made her theatre debut in 2010 in Nicolas Bedos's Promenade de santé. The short film De moins en moins (2008) marked her debut as a filmmaker. Her feature film directorial debut is The Adopted (2011). Respire (2014), her second production as a director, was screened in the Critics' Week section at the 2014 Cannes Film Festival. She made her singing debut with a studio album, En attendant (Waiting For You), in 2011.