Its collections range from ancient Egypt antiquities to the Modern art period and make the museum one of the most important in France outside Paris, notably for its paintings and drawings holdings.

However the majority of the present holdings come from the private collection of Christophe-Paul de Robien (1698–1756), a president of the Parlement of Rennes, which was at the time of the Revolution one of the largest of its kind in Europe.

Primitive and Renaissance painting is represented with works by Paris Bordone, Paolo Veronese, Leandro Bassano, Maarten van Heemskerck and of the School of Fontainebleau.

20th-century painting and sculpture, notably the 1900-1950 period with Fauvism, cubism, abstraction and surrealism, is well represented with works by Raoul Dufy, Pablo Picasso, Robert Delaunay, Juan Gris, Alberto Magnelli, František Kupka, René Iché, Yves Tanguy and Nicolas de Staël.

Artworks in this section include drawings by Filippo Lippi, Leonardo da Vinci, Botticelli, Donatello, Domenico Ghirlandaio, Michelangelo, Giovanni Bellini, Albrecht Dürer, Corregio, Pontormo, Giulio Romano, Parmigianino, Nicolo dell'Abbate, Federico Barocci, Rubens, Pietro da Cortona, Simon Vouet, Pierre Puget, Rembrandt, Salvator Rosa, Antoine Watteau, Sebastiano Ricci, Pierre Bonnard, Maurice Denis, Édouard Vuillard and Pablo Picasso.