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Byrne's acting career began at the Focus Theatre in Dublin before he joined London's Royal Court Theatre in 1974. His screen debut came in the Irish drama serial The Riordans and the spin-off show Bracken. He went on to star in such films as Defence of the Realm (1986), Lionheart (1987), Miller's Crossing (1990), Little Women (1994), Dead Man (1995), The Usual Suspects (1995), The Man in the Iron Mask (1998), Enemy of the State (1998), Vanity Fair (2004), The 33 (2015), and Hereditary (2018). He co-wrote The Last of the High Kings (1996) and produced In the Name of the Father (1993).

For his Broadway work, Byrne has received two nominations for the Tony Award for Best Actor in a Play for his roles in the Eugene O'Neill plays A Moon for the Misbegotten (2000) and Long Day's Journey into Night (2016). For his television work, Byrne has received two nominations for the Primetime Emmy Award for Outstanding Lead Actor in a Drama Series for his role as Paul Weston in the HBO drama series In Treatment (2008–2010). He also received a Golden Globe Award. His other notable television roles include Vikings (2013), Maniac (2018), and War of the Worlds (2019–2022).