In January 1938, Guggenheim opened a gallery for modern art in London featuring Jean Cocteau drawings in its first show, and began to collect works of art. Guggenheim often purchased at least one object from each of her exhibitions at the gallery. After the outbreak of World War II, she purchased as much abstract and Surrealist art as possible.  Her first gallery was called Guggenheim Jeune, the name being ingeniously chosen to associate the epitome of a gallery, the French Bernheim-Jeune, with the name of her own well known family. The gallery on 30 Cork Street, next to Roland Penrose's and E. L. T. Mesens' show-case for the Surrealist movement, the London Gallery, proved to be successful, thanks to many friends who gave advice and who helped run the gallery. Marcel Duchamp, whom she had known since the early 1920s, when she lived in Paris with her first husband Laurence Vail, had introduced Guggenheim to the art world; it was through him that she met many artists during her frequent visits to Paris. He taught her about contemporary art and styles, and he conceived several of the exhibitions held at Guggenheim Jeune.  The Cocteau exhibition was followed by exhibitions on Wassily Kandinsky (his first one-man-show in England), Yves Tanguy, Wolfgang Paalen and several other well-known and some lesser-known artists. Peggy Guggenheim also held group exhibitions of sculpture and collage, with the participation of the now classic moderns Antoine Pevsner, Henry Moore, Henri Laurens, Alexander Calder, Raymond Duchamp-Villon, Constantin Brancusi, Jean Arp, Max Ernst, Pablo Picasso, Georges Braque and Kurt Schwitters. She also greatly admired the work of John Tunnard (1900-1971) and is credited with his discovery in mainstream international modernism.

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She also greatly admired the work of John Tunnard (1900-1971) and is credited with his discovery in mainstream international modernism.