Theo James made his debut in the 2010 comedy-drama film ‘You Will Meet a Tall Dark Stranger’ directed by Woody Allen. The film received a mixed response from critics. That same year, he also made his first television appearance in the British two-part drama mini-series A ‘Passionate Woman’ where he played the role of Alex "Craze" Crazenovski. In 2011, he starred as ‘James’ in the British coming-of-age teen comedy film ‘The Inbetweeners Movie’ directed by Ben Palmer. The film saw mixed reviews upon release and was a major financial success, grossing over $88 million on a budget of 4.9 million. The following year, he appeared in the American action horror film ‘Underworld: Awakening’ directed by Måns Mårlind and Björn Stein. Despite being panned by critics, the film was a financial success. In 2014, he got his breakthrough role as Tobias "Four" Eaton in the American social science fiction action film ‘Divergent’ directed by Neil Burger. The film opened to a mixed reception and did decent business at the box office. James also became a recipient of 2 ‘Teen Choice Awards’ for his performance in the film
In 2015, he reprised his role as Tobias "Four" Eaton in ‘The Divergent Series: Insurgent,’ the sequel to the 2014 film ‘The Divergent.’ The film received mixed reviews and was a financial success. That same year, he also appeared in the American drama film ‘The Benefactor’ directed by Andrew Renzi. The film saw mostly negative reviews upon release. He returned to play Tobias "Four" Eaton in ‘The Divergent Series: Allegiant,’ the third and final part in ‘The Divergent Series.’ The film was panned by critics and was a box office bomb. That same year, he also reprised his role as ‘David’ in ‘Underworld: Blood Wars,’ the sequel to the 2012 film ‘Underworld: Awakening.’ Even though the film opened to negative reviews, it managed to emerge as a financial success. In 2018, he joined the cast of the American adult animated dark fantasy action streaming television series ‘Castlevania’ where he voiced the character ‘Hector.’ The series aired its final episode in 2021.
He played the role of ‘Michael’ in the 2018 political thriller film ‘Backstabbing for Beginners’ directed by Per Fly. The film received a lukewarm response from critics. He next appeared in films like ‘Zoe’ (2018), ‘How It Ends’ (2018), ‘London Fields’ (2018), ‘Lying and Stealing’ (2019), and ‘Archive’ (2020). James was last seen in the adult animated dark fantasy film ‘The Witcher: Nightmare of the Wolf’ directed by Kwang Il Han. The film received mostly positive reviews from critics. He is all set to appear in the upcoming period drama film ‘Mr. Malcolm's List’ directed by Emma Holly Jones.