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Hüller made her film debut in 1999. She would go on to win Silver Bear for Best Actress for her performance as a woman based on the case of Anneliese Michel in Hans-Christian Schmid's drama Requiem (2006) and the Silver Bear for Best Leading Performance for playing a female soldier disguised as a man in Markus Schleinzer's drama Rose (2026). She also took leading roles in Maren Ade's comedy Toni Erdmann (2016) and Frauke Finsterwalder's historical black comedy Sisi & I (2023).

She gained international recognition in 2023 for her starring roles in Justine Triet's legal drama Anatomy of a Fall and Jonathan Glazer's Holocaust drama The Zone of Interest. Her performance in the former won a César Award and earned her an Academy Award nomination for Best Actress. In 2026, she appeared in the science-fiction comedy-drama Project Hail Mary, the Paweł Pawlikowski drama Fatherland, and the Alejandro G. Iñárritu satire Digger.