In 1959 she appeared as Ophelia in a TV production of Hamlet. For the James Bond film From Russia with Love (1963) she provided the uncredited voice of Tatiana Romanova, played by Daniela Bianchi. Jefford provided additional voice work in later Bond films, dubbing Molly Peters in Thunderball (1965) and Caroline Munro in The Spy Who Loved Me (1977). Her first major film role was as Molly Bloom in Ulysses (1967), for which she was nominated for a British Academy Award. This was followed by A Midsummer Night's Dream (1968), The Bofors Gun (1968), The Shoes of the Fisherman (1968) and Lust for a Vampire (1971) She played Magda Goebbels in Hitler: The Last Ten Days (1973). Other films include Nelly's Version (1983), Fellini's And the Ship Sails On (E la nave va) (1983), Claudia (1985), When the Whales Came (1989), The Saint, Roman Polanski's The Ninth Gate (1999) and Terence Davies's The Deep Blue Sea. In 2013, she played Sister Hildegard, a small but crucial part, in Stephen Frears's Philomena with Judi Dench and Steve Coogan.