In 2009, her breakthrough came with Le Bel Âge in which she played opposite Michel Piccoli, and for which she won an actress prize at the Festival international des jeunes réalisateurs de Saint-Jean-de-Luz. Her work in Qu'un seul tienne et les autres suivront, directed by Léa Fehner, won her the Prix Lumière best actress newcomer award, then the Étoile d'or de la presse de la révélation féminine in 2010.
In 2013 she appeared in a new screen version of Denis Diderot's The Nun.[4] She received two nominations for her outstanding performance for her role as the nun Suzanne, including winning the best actress award in the 4th Magritte Awards. In 2014 she had main roles for the films Eden and Tokio Fiancée for which she won Best Actress.
In 2016, she played a recurring role as Céline Delorme in the French political thriller television series The Bureau directed by Éric Rochant.
In 2018, Pauline appeared in her first English-language movie, Old Boys, in which she plays the main role of Agnes.
In 2020, she played the lead role in the Belgian apocalyptic sci-fi drama thriller streaming television series Into the Night.