Hurt came to prominence for his role as Richard Rich in the film A Man for All Seasons (1966) and gained BAFTA Award nominations for his portrayals of Timothy Evans in 10 Rillington Place (1971) and Quentin Crisp in television film The Naked Civil Servant (1975) – winning his first BAFTA for the latter. He played Caligula in the BBC TV series I, Claudius (1976). Hurt's performance in the prison drama Midnight Express (1978) brought him international renown and earned Golden Globe and BAFTA Awards, along with an Academy Award nomination. His BAFTA-nominated portrayal of astronaut Kane, in the science-fiction horror film Alien (1979), yielded a scene where an alien creature burst out of his chest. It has been named by several publications as one of the most memorable moments in cinema history.
Hurt earned his third competitive BAFTA, along with his second Oscar and Golden Globe nominations, as John Merrick in David Lynch's biopic The Elephant Man (1980). Other significant roles during the 1980s included Bob Champion in biopic Champions (1984), Mr. Braddock in the Stephen Frears drama The Hit (1984), Winston Smith in Nineteen Eighty-Four (1984) and Stephen Ward in the drama depicting the Profumo affair, Scandal (1989). Hurt was again BAFTA-nominated for his work in Irish drama The Field (1990) and played the primary villain, James Graham, in the epic adventure Rob Roy (1995). His later films include the Harry Potter film series (2001–11), the Hellboy films (2004 and 2008), supernatural thriller The Skeleton Key (2005), western The Proposition (2005), political thriller V for Vendetta (2005), sci-fi adventure Indiana Jones and the Kingdom of the Crystal Skull (2008) and the Cold War espionage film Tinker Tailor Soldier Spy (2011). Hurt reprised his role as Quentin Crisp in An Englishman in New York (2009), which brought his seventh BAFTA nomination. He portrayed the War Doctor in BBC TV series Doctor Who in 2013.
Hurt was regarded as one of Britain's finest actors; director David Lynch described him as "simply the greatest actor in the world". He possessed what was described as the "most distinctive voice in Britain", likened by The Observer to "nicotine sieved through dirty, moonlit gravel". His voice acting career encompassed films such as Watership Down (1978), The Lord of the Rings (1978), The Plague Dogs (1982), The Black Cauldron (1985) and Dogville (2003), as well as BBC TV series Merlin (2008–2012). In 2012, he was honoured with the Lifetime Achievement BAFTA Award, in recognition of his "outstanding contribution to cinema". He was knighted in 2015 for his services to drama.
- This Is My Street (1964; Warner-Pathé Distributors) - Charlie
- Even Cowgirls Get the Blues (1993; Fine Line Features) - The Countess
- Thumbelina (1994; Don Bluth Entertainment/Warner Bros.) - Mr. Mole
- Second Best (1994; Warner Bros.) - Uncle Turpin
- Contact (1997; Warner Bros.) - S.R. Hadden
- Lost Souls (2000; New Line Cinema) - Father Lareaux
- Harry Potter and the Philosopher's Stone (2001; Warner Bros.) - Garrick Ollivander
- V for Vendetta (2005; Warner Bros./Vertigo (DC Comics)) - Adam Sutler
- Harry Potter and the Deathly Hallows – Part 1 (2010; Warner Bros.) - Garrick Ollivander
- Harry Potter and the Deathly Hallows – Part 2 (2011; Warner Bros.) - Garrick Ollivander
- The Legend of Tarzan (2016; Warner Bros.) (was deleted)