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He was introduced to mainstream international audiences through his breakthrough performance as Fredrick Zoller, a Nazi German war hero in Quentin Tarantino's Inglourious Basterds (2009), and appearances in films like The Bourne Ultimatum (2007), The Fifth Estate (2013), and A Most Wanted Man (2014). Brühl received widespread critical acclaim and further recognition for his portrayal of former Formula 1 driver Niki Lauda in the biographical film Rush (2013), for which he earned nominations including the Golden Globe Award for Best Supporting Actor, the Critic's Choice Award for Best Supporting Actor, the Screen Actors Guild Award for Best Supporting Actor and the BAFTA Award for Best Actor in a Supporting Role.

In the Marvel Cinematic Universe, Brühl portrays Helmut Zemo in Captain America: Civil War (2016) and the Disney+ series The Falcon and the Winter Soldier (2021). He also starred as Dr. Laszlo Kreizler in the Emmy- and Golden Globe-nominated period drama television series The Alienist (2018–2020), for which he earned a nomination for the Golden Globe Award as Best Actor in a Television Motion Picture at the 76th Golden Globe Awards in 2018.