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He started his career portraying Mike Young in the Australian television series Neighbours (1986–1989). Pearce received international attention for his breakout role in The Adventures of Priscilla, Queen of the Desert (1994). Subsequently, he starred as Ed Exley in Curtis Hanson's crime noir L.A. Confidential (1997) and a man suffering short-term memory loss in Christopher Nolan's psychological thriller Memento (2000).

He also acted in The Time Machine (2002), Bedtime Stories (2008), The Road (2009), The Hurt Locker (2009), The King's Speech (2010), and Lawless (2012). He portrayed Peter Weyland in Prometheus (2012) and Alien: Covenant (2017), Aldrich Killian in the Marvel action film Iron Man 3 (2013) and William Cecil in the biopic Mary Queen of Scots (2018). In Australian cinema, Pearce has acted in The Proposition (2005), Animal Kingdom (2010), and The Rover (2014). For his performance in The Brutalist(2024), he received a nomination for the Academy Award for Best Supporting Actor.

Since 2012, he has played the title role in the TV adaptations of the Jack Irish stories by Australian crime writer Peter Temple. Pearce starred in the HBO miniseries Mildred Pierce (2011) and Mare of Easttown. The former won him a Primetime Emmy Award for Outstanding Supporting Actor.