Phillipe Halsman had his first success in America when the cosmetics firm Elizabeth Arden used his image of model Constance Ford against the American flag in an advertising campaign for "Victory Red" lipstick. A year later in 1942 he found work with Life, photographing hat designs, one of which, a portrait of a model in a Lilly Daché hat, was his first of the many covers he would do for Life.
In 1941 Halsman met the surrealist artist Salvador Dalí and they began to collaborate in the late 1940s. The 1948 work Dali Atomicus explores the idea of suspension, depicting three cats flying, a bucket of thrown water, and Salvador Dalí in mid air. The title of the photograph is a reference to Dalí's work Leda Atomica which can be seen in the right of the photograph behind the two cats. Halsman reported that it took 28 attempts to be satisfied with the result. Halsman and Dali eventually released a compendium of their collaborations in the 1954 book Dali's Mustache, which features 36 different views of the artist's distinctive mustache. Another famous collaboration between the two was In Voluptas Mors, a surrealistic portrait of Dali beside a large skull, in fact a tableau vivant composed of seven nudes. Halsman took three hours to arrange the models according to a sketch by Dali. A version of In Voluptas Mors was used subtly in the poster for the film The Silence of The Lambs, and recreated in a poster for the film The Descent.
In 1947, he made what was to become one of his most famous photos of a mournful Albert Einstein, who during the photography session recounted his regrets about his role in the United States pursuing the atomic bomb. The photo would later be used in 1966 on a U.S. postage stamp and in 1999, on the cover of Time, when Time dubbed Einstein as "Person of the Century."