Dalí visited Paris in the 1920s, meeting Spanish painter Joan Miro, who introduced him to surrealism. In 1929, he co-wrote the screenplay of the first surrealist film, Un Chien Andalou with the director Bunuel and in the same year formally became a member of the surrealists. His talent for self-publicity soon made him the most prominent member of the group.

During the 1930s, Dalí painted his best-known surrealist works, such as The Persistence of Memory (1931). He developed a style that he termed "paranoiac-critical", using a meticulously realistic technique to create "hand-painted dream photographs" with a hallmark imagery of hallucinatory decay, molten watches, burning giraffes and human chests of drawers.

In 1934, he married Gala, the former wife of French poet Paul Eluard, who became his muse. Dalí participated in several surrealist group shows in the 1930s, despite disagreements with surrealism's founder, André Breton. In 1936, at the International Surrealist Exhibition in London, he gave a lecture dressed in a diver's suit.

Dalí finally broke with the surrealists in 1939 after declaring his support for Spanish dictator Franco. He had in any case moved away from surrealism to a more naturalistic style, influenced by his admiration for renaissance art. In 1939, he moved to the United States, where he exhibited widely, wrote a fictionalised autobiography, The Secret Life of Salvador Dalí, and developed his talent for self-publicity. His work at this time included designing stage sets for ballets, a project with Walt Disney and a dream sequence for Alfred Hitchcock's film Spellbound (1945).

In 1948, Dalí returned to Spain but made frequent visits to New York. He now began to produce a series of religious paintings, notably Christ of St John of the Cross (1951). In 1979, a large retrospective exhibition of his work was mounted at the Georges Pompidou Centre, Paris.