When Edouard André died, Nélie Jacquemart completed the decoration of the Italian Museum and travelled in the Orient to add more precious works to the collection.

Faithful to the plan agreed with her husband, she bequeathed the mansion and its collections to the Institut de France as a museum, and it opened to the public in 1913.

Dominated by a coffer ceiling attributed to Mocetto, paintings by Mantegna, Bellini or Carpaccio recreate the typical setting of a Venetian Palazzo.

The museum features works by Élisabeth-Louise Vigée Le Brun, Bellini, Francesco Botticini, Luca Signorelli, Cima da Conegliano, Pietro Perugino, Neri di Bicci, Vittore Crivelli, Luca della Robbia, Paolo Uccello, Canaletto, Jean-Marc Nattier, Alfred Boucher, Quentin Massys, Rembrandt, Anthony van Dyck, Frans Hals, Giovanni Battista Tiepolo, Jacques-Louis David, Franz Xaver Winterhalter, Thomas Lawrence, Joshua Reynolds, Thomas Gainsborough, Gian Lorenzo Bernini, Sandro Botticelli, Andrea Mantegna, Jean-Honoré Fragonard, and Jean-Baptiste-Siméon Chardin.

The final banquet of the 2002 film The Count of Monte Cristo by Kevin Reynolds was shot in a replica of the Grand Salon and the Honour Staircase of the Musée Jacquemart-André, but without the dividing wall in-between.