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Byrne has worked with numerous acclaimed directors and popular actors on the silver screen, including for Martin Scorsese in Gangs of New York; Braveheart, directed by and starring Mel Gibson; The Sum of All Fears, with Ben Affleck; Battlefield Earth: A Saga of the Year 3000, with John Travolta; Proof of Life, opposite Russell Crowe and Meg Ryan; Tomorrow Never Dies, with Pierce Brosnan; Apt Pupil, with Brad Renfro and David Schwimmer; The Saint, with Val Kilmer and Elizabeth Shue; Steven Spielberg's Indiana Jones and the Last Crusade, starring Harrison Ford and Sean Connery; A Bridge Too Far, with Michael Caine, Gene Hackman and Anthony Hopkins; The Musketeer, with Catherine Deneuve and Stephen Rea, and the crime/drama Gunshy, with William L. Petersen. Foreign films include The Eagle Has Landed, with Robert Duvall, Michael Caine and Donald Sutherland; The Island on Bird Street; the 1994 drama Nostradamus; Buster and The Good Father, opposite Anthony Hopkins. He was also cast in the leading role of the 19th century national hero, Mauã, in the Brazilian historical epic, Mauã: O Imperador e o Rei.

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His U.S. television appearances include the made-for-television-movies Deadly Voyage with Omar Epps, The Infiltrator and The Plot to Kill Hitler, as well as the miniseries The Mists of Avalon, with Anjelica Huston, Joan Allen and Julianna Margulies, and Ellis Island. He also guest starred on ABC's live action series, Dinotopia.

Byrne also has been a strong presence on British television, having starred in the television film Holocaust on Trial and appeared in other television movies such as The Crooked Man, Sunday, Hornblower, Imogen's Face, Sharpe's Honour, Sharpe's Enemy, Sharpe's Company, The Orchid House, The Happy Valley, The Pale Horse, Devil's Advocate, A Few Short Journeys of the Heart, Running Later, Advocates I, Shake Hands Forever, Oedipus the King and Two Gentlemen of Verona. His miniseries credits include Heat of the Sun, No Bananas, Smiley's People, Oliver's Travels and a major role in Lord Mountbatten: The Last Viceroy. Additionally he starred in the U.K. series A Sort of Innocence and guest starred on Helen West, Ultimate Force, Saracen, The Vice and Between the Lines. On stage Byrne has performed in Filumena for The Peter Hall Company, Phaedre, Kafka's Dick, Hamlet, Duchess of Malfi, Man and Superman, and in numerous productions for the Royal National Theatre and The Royal Court. His most recent stage performance was in the title role of The Mayor of Zalamea.

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