The collection of musical instruments includes about 70 items dating from the period between the 17th and 20th centuries. Items made in Neuchâtel are exhibited side-by-side with instruments of great importance from elsewhere. Among these, the historic harpsichord built in 1632 at Antwerp by Johannes Ruckers the Younger, and restored in Paris during the 18th century, is still played and appreciated by specialists in this instrument. Other outstanding items include the guitar presented by the lute-maker George Stauffer to the Empress Marie-Louise in 1810, and the lyre-guitar made by Augustin Claudot in 1815 which belonged to Mademoiselle Robert, sister of the painter Léopold Robert.

The Museum also holds 300 items of furniture, mostly made in Switzerland and Neuchâtel, which afford interesting insights into the furnishing tastes of the Neuchâtel population between the 17th and 20th centuries.