Harbour began acting professionally on Broadway in 1999, in the revival of The Rainmaker. He then made his television debut that same year in an episode of Law & Order, playing a waiter. He appeared again in 2002 in an episode of Law & Order: Special Victims Unit, playing a child murderer. Harbour portrayed the recurring role of MI6 Agent Roger Anderson in the ABC series Pan Am. In 2005, he was nominated for a Tony Award for his performance in a production of Who's Afraid of Virginia Woolf?.
Harbour is also known for his role as CIA Agent Gregg Beam in Quantum of Solace, as Shep Campbell in Revolutionary Road, and as Russell Crowe's source in State of Play. He also received praise for his role as spree killer Paul Devildis in a 2009 episode of Law & Order: Criminal Intent. Harbour's other film credits include Brokeback Mountain, The Green Hornet, End of Watch, and Between Us. In 2013, he played a small role of a head doctor in the television series Elementary. From 2012 to 2014, he also played the recurring role of Elliot Hirsch in The Newsroom.
In 2014, Harbour played the recurring character of Dr. Reed Akley in the first season of the historical drama series Manhattan. He currently plays the lead role of Chief Jim Hopper in the Netflix science fiction horror series Stranger Things. For his role as Hopper, Harbour has received nominations for the Primetime Emmy Award for Outstanding Supporting Actor in a Drama Series (2017 and 2018) and the Golden Globe Award for Best Supporting Actor – Series, Miniseries or Television Film (2018). Harbour has won a Screen Actors Guild Award for Outstanding Performance by an Ensemble in a Drama Series (2017) along with the rest of the cast.
Harbour will portray the title character in the film reboot Hellboy (2019).
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