Jaffrey is well known in both Britain and his native India. He was cast as Hamidullah in David Lean's A Passage to India and played the Nawab of Mirat in Granada Television's The Jewel in the Crown. He is also known for My Beautiful Laundrette.  Jaffrey was the first Asian actor to be awarded an OBE for services to drama in 1995.

 His career began in the mid-1950s with All India Radio. In Delhi, Jaffrey founded the Unity Theatre, the staple of which was English plays. He got a Fulbright Scholarship to attend Catholic University in Washington, D.C. Jaffrey was the first Indian to tour the United States performing Shakespeare and also the first Indian to appear on Broadway, playing Professor Godbole in a production of A Passage to India in 1958. Notably, he was primarily playing white charaters, including in Witness for the Prosecution.  He moved from the United States to the UK when his marriage to Madhur Jaffrey ended in divorce. He worked for the BBC World Service and as a shop assistant in Harrod's before he was able to earn his living in his profession.