The museum has a considerable collection of paintings by Vincent van Gogh, such as The Potato Eaters, Cafe Terrace at Night and On the Threshold of Eternity, 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 is named after 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, designed by Henry van de Velde opened. The sculpture garden was added in 1961 and the new exhibition wing, designed by Wim Quist, opened in 1977.
The Kröller-Müller Museum is also famous for its large sculpture garden, within the forest park, of more than 75 acres (300,000 m2) and one of the largest in Europe, with a fine collection of modern and contemporary sculptures. The garden reflects Helene Kröller-Müller's conception of a symbiosis between art, architecture and nature. The collection includes works by Auguste Rodin, Henry Moore, Jean Dubuffet, Mark di Suvero, Lucio Fontana, Claes Oldenburg, Fritz Wotruba, Joep van Lieshout and many more.
The Jachtslot St Hubertus is a building designed as the residence in the hunting season for the Kröller-Müller family by the Dutch architect Berlage. The building is located near the Kröller-Müller Museum in the centre of the National Park De Hoge Veluwe.