In addition to Shakespeare, during a six decade career, Olivier played many other roles on stage and screen. On stage his more than 120 roles including Richard III, Macbeth, Romeo, Hamlet, Uncle Vanya, and Archie Rice in The Entertainer. He appeared in nearly 60 films, including William Wyler's Wuthering Heights (1939), Alfred Hitchcock's Rebecca (1940), Stanley Kubrick's Spartacus (1960), and Joseph L. Mankiewicz's Sleuth (1972). His other Shakespeare roles for the cinema were as Orlando in As You Like It (1936) and the lead in Othello (1965), with virtually the entire cast from the production at the Old Vic of the National Theatre Company, of which he was then artistic director. He had earlier filled the same post at the Old Vic after the war. The largest stage in the National Theatre building was later named after him.

Olivier retired from the stage in 1973, but his work on screen continued. For television, he starred in Long Day's Journey into Night (1973), The Merchant of Venice (1973), Cat on a Hot Tin Roof (1976), Brideshead Revisited (1981), and King Lear (1983), among others. The later cinema films included John Schlesinger's Marathon Man (1976) and Richard Attenborough's A Bridge Too Far (1977). Continuing to act until the year before his death in 1989, he was married three times, to actresses Jill Esmond, Vivien Leigh, and Joan Plowright.

Actor Spencer Tracy stated that Olivier was "the greatest actor in the English-speaking world". He is regarded by some to be the greatest actor of the 20th century, in the same category as David Garrick, Richard Burbage, Edmund Kean and Henry Irving in their own centuries. Olivier's AMPAS acknowledgments are considerable: twelve Oscar nominations, with two awards (for Best Actor and Best Picture for the 1948 film Hamlet), plus two honorary awards including a statuette and certificate. He was also awarded five Emmy awards from the nine nominations he received. Additionally, he was a three-time Golden Globe and BAFTA winner.