He played Ian Curtis in 24 Hour Party People (2002), Micheletto Corella in The Borgias (2011–2013), Fifield in Prometheus (2012), Solomon Lane in Mission: Impossible – Rogue Nation (2015) and Mission: Impossible – Fallout (2018), Philip in Possum (2018), William Gascoigne in The King (2019), Henry Peter Teague / Peter Morley in The Stranger (2022), and Jacob Pearce in Paris Has Fallen (2024).

[11] In 2009, he played corrupt Detective Inspector Bob Craven in Channel 4's critically acclaimed Red Riding trilogy,[11] and as photographer Anton Blair in Dean Cavanagh's comedy series, Svengali.

[13] In the BBC TV drama Five Daughters (2010), Harris portrayed Brian Tobin, co-founder of the drug treatment facility, The Iceni Project, based in Suffolk.

[2][16][17] He also played Joss Merlyn in the poorly received BBC adaptation of Jamaica Inn, which became a subject of controversy and made national news over its mumbling cast and other sound problems.

[18][19] He appears as the disfigured former soldier turned terrorist mastermind Jacob Pearce in the 2024 French/British action thriller series Paris Has Fallen.

[2] In 2014, Harris played Mick Santino in Deliver Us from Evil (2014), directed by Scott Derrickson and based upon the 2001 novel "Beware the Night" by Ralph Sarchie and Lisa Collier Cool.

[11] In 2015, Harris appeared as Solomon Lane in Mission: Impossible – Rogue Nation, directed by Christopher McQuarrie, and as Macduff in Justin Kurzel's Macbeth earning another BIFA nomination.

[31] Harris made a cameo appearance as a clown in a music video for the Norwich band the Black Sharks' debut album titled Lose Control, directed by Myhill (evidently filmed at the same time as The Fabulous Bilsons).