The print collection was begun in the first half of the 19th century; it grew between 1850 and 1950 thanks to major donations and numerous purchases. It comprises over 22,000 folios dating from the 16th century until modern times. The collection was originally split between interpretative and original engraving, with a major focus on the Neuchâtel engravers (François Forster and the Girardet dynasty, among others) as well as the minor Swiss masters and representatives of the Italian, English, German and (especially) French schools.

Since 1950, acquisitions have favoured contemporary artists (mainly Swiss), proving that prints were still very much alive in the art world of the 20th century. Thanks to Aimé Montandon's bequest of his studio collection, this artist is represented by almost all of his engraved work, supplemented by thousands of drafts and studies.

Between 2000 and 2012, the Jeunet donation added several hundred items to the collection, including works by artists from Neuchâtel (Evrard, Lermite, Mosset and others) and elsewhere in Switzerland (Gottfried Honegger); international artists such as Franck Badur, Aurélie Nemours and François Morellet are also represented.