The museum has a considerable collection of paintings by Vincent van Gogh, such as The Potato Eaters, Cafe Terrace at Night and Sorrowing Old Man ('At Eternity's Gate'), making it the second-largest collection of Van Gogh paintings in the world (after the Van Gogh Museum in Amsterdam).
Apart from the Van Gogh paintings other highlights include works by Piet Mondrian, Georges-Pierre Seurat, Odilon Redon, George Braque, Paul Gauguin, Lucas Cranach, James Ensor, Juan Gris, Pablo Picasso, etc.
The museum was founded by Helene Kröller-Müller, an avid art collector who was one of the first to recognize Van Gogh's genius and collect his works. In 1935, she donated her whole collection to the state of the Netherlands. In 1938, the museum, which was designed by Henry van de Velde, opened to the public. The sculpture garden was added in 1961 and the new exhibition wing, designed by Wim Quist, opened in 1977.