She gained wider recognition for her 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.

Additionally, she starred in Chris Weitz's 2018 drama Operation Finale, telling the story of the capture of Nazi Adolf Eichmann.

[11] Laurent's breakthrough role came in 2006, when she played a sullen 19-year-old who longed for her lost twin brother, in Philippe Lioret's Don't Worry, I'm Fine.

[12][13] In a review for Variety, Ronnie Scheib praised Laurent and wrote that she, "makes her vibrant character's downward spiral totally believable without indulging in moody sullenness".

[15] Laurent then starred in the Franco-Belgian Dikkenek, a comedy directed by Olivier Van Hoofstadt that has attained a cult film over the years owing to its Belgian-style humour, in which she co-starred alongside Marion Cotillard, Jérémie Renier, Jean-Luc Couchard and Dominique Pinon.

[21] Laurent was scheduled to direct her first play, Mi-cuit cœur pistache (the name of a dessert she particularly likes) in January 2009 at the Théâtre Marigny in Paris.

She had to abandon the project when she was cast as Shosanna Dreyfus, a Parisian who seeks revenge on Nazis in the Quentin Tarantino film Inglourious Basterds, alongside Brad Pitt, Diane Kruger and Christoph Waltz.

[30] In 2010, Laurent starred in The Round Up, a French film directed by Roselyne Bosch, and produced by Alain Goldman, alongside Jean Reno, Sylvie Testud, and Gad Elmaleh.

Based on the true story of a young Jewish boy, the film depicts the Vel' d'Hiv Roundup, the mass arrest of Jews by French police who were Nazi accomplices in Paris in July 1942.

[34] Laurent had also planned another feature film, Putain de pluie!, produced by Alain Attal's Productions du Trésor, whose script she co-wrote with Morgan Perez and which she intended to direct.

"[37][38] Mick LaSalle of San Francisco Chronicle called it a "role with great technical demands" and praising Laurent wrote, "she's extremely subtle and reserved ... "The Concert" constitutes a breakthrough for her, in that it unlocks her emotional floodgates".

[40] In 2011, she teamed with Mike Mills, appearing opposite Ewan McGregor and Christopher Plummer in Beginners, a comedy drama that marked Laurent's second English-speaking role in Hollywood.

Loosely based on Mills' own life, the film depicts the story of a father coming out of the closet at the age of 75 after the death of his wife of 45 years.

[42][43] Laurent then starred opposite Jeremy Irons in Night Train to Lisbon, a 2013 drama film based on the novel of the same name directed by Bille August.

[44] Jessica Kiang of Indie Wire noted that Laurent was "given less to do" but lauded her performance writing that she, "makes the most of her truncated screen time".

[45] Laurent appeared in the Louis Leterrier's 2013 caper film Now You See Me as a French Interpol agent who investigates the bank theft alongside Mark Ruffalo and an ensemble cast.

The film was a major commercial success grossing over 351.7 million dollars, receiving mixed reviews but praise for the performances of the entire cast.

[50] In 2014, Laurent appeared in Aloft, a 2014 drama film written and directed by Claudia Llosa, alongside Jennifer Connelly and Cillian Murphy.

Laurent voiced Mary Katherine in Blue Sky Studios' Epic, and Disgust in Pixar's Inside Out in the French dubs of the animated films.

[53] The Hollywood Reporter wrote, "Boomerang is a solid if somewhat conventionally made whodunit that benefits from a strong cast and a plot that hooks you for most of the running time.

Laurent was announced to direct The Nightingale, an adaptation of novel of the same name by Kristin Hannah, which was set to star Elle and Dakota Fanning.

Produced by Joel Shearer, the album contains twelve songs, five of which are co-written and co-produced by Irish folk musician Damien Rice.

[76] Laurent revealed that spending time at musician Damien Rice's home in Ireland, while working on her 2011 album, inspired her to maintain a compost heap and eat organic food.