In 2004, he starred in Jean-Pierre Jeunet’s A Very Long Engagement and won a César Award for Most Promising Actor for his performance.

In 2007, he appeared on the cover of the January issue of French Vogue with supermodel Doutzen Kroes. Ulliel later was chosen as the face of Chanel for its new men’s fragrance, Bleu de Chanel. The film for the campaign was directed by Academy Award-winning director Martin Scorsese and debuted in August 2010.

Ulliel dated French actress Cécile Cassel from 2005 to 2007. Had a brief relationship with Charlotte Casiraghi in 2007 and dated Jordane Crantelle from 2008 to 2013.

Since 2013, Ulliel has been in a relationship with French model-singer Gaëlle Piétri. On November 9, 2015, it was announced that the couple were expecting their first child together. The birth of the couple’s son was announced on February 9, 2016.

He portrayed French fashion designer Yves Saint Laurent in the 2014 biopic film Saint Laurent, which earned him a Lumières Award for Best Actor and a César Award for Best Actor nomination.

In 2016, he appeared in two films: the lead role in Xavier Dolan’s It’s Only the End of the World; and in Stephanie Di Giusto’s The Dancer, an unconventional biopic of American dancer Loie Fuller. He will also star in Guillaume Nicloux’s Les Confins du Monde, opposite Gérard Depardieu.

In 2017, he was nominated for the Jury Prize for Best Actor at the Riviera International Film Festival for his role in Xavier Dolan’s It’s Only the End of the World alongside co-star Vincent Cassel. The film was nominated for the Grand Jury Prize for Best Picture as well.