Initiated in 1816, the collection of paintings now comprises 2,700 canvases from the 16th to the 21st centuries. Neuchâtel art is a primary focus of this collection, but it also includes Swiss and European creative work as well as Russian and American art.

Among most prominent artists are the "Carnation Master", Maximilien de Meuron, Léopold Robert, Alexandre Calame, Albert Anker, Cuno Amiet, Ferdinand Hodler, Félix Vallotton and Kees Van Dongen: the list could go on. The bequest of Yvan and Hélène Amez-Droz, the cornerstone of this collection, features works by several Impressionists including the famous Studio Boat by Claude Monet (1876).

Gérard Schneider, Günther Förg, Olivier Mosset, Grégoire Müller, Guy Oberson and many other Swiss and international artists are represented by works exemplifying the various movements that emerged in the 20th and 21st centuries, spanning abstract and figurative art. Finally, the extensive Jeunet Donation focuses on lyrical and geometric abstraction.