The Gallery hosts Romania’s premier collection of European art. In time, the Picture Gallery of King Carol I was complemented with works from various the Ioan and Dr. Nicolae Kalinderu, Toma Stelian, Anastasie Simu, and Al. Saint-Georges collections alongside paintings from the Bucharest Municipal Picture Gallery. After 1950 the collection continued to grow through donations and acquisitions.

Art collector and critic Krikor H. Zambaccian (1889-1962) put together one of the richest and most valuable private collections in Romania. In the 1940s Zambaccian had the house purpose built so as to enable him to display the paintings, sculptures, prints and drawings and furniture he had acquired over more than half a century. Both the collection and the house were donated by him to the Romanian State in 1947.
In celebration of his deed, Zambaccian was made a member of the Romanian Academy.
The collector’s portfolio of Romanian artists offers a brief but dense overview of modern Romanian art, covering representative paintings by founding figures like Theodor Aman, Nicolae Grigorescu, Ioan Andreescu, classical modernists like Ștefan Luchian, Nicolae Tonitza, Theodor Pallady and Gheorghe Petrașcu, and post-war figurative painters like Corneliu Baba, Alexandru Phoebus and Horia Damian. Sculptures by Brâncuși, Milița Petrașcu, Oscar Han and Cornel Medrea reflect Zambaccian’s preference for a more traditional vein of modernism. To create a context for Romanian art and enhance his prestige, Zambaccian also acquired works by Cézanne, Picasso, Matisse, Bonnard, Utrillo, and Marquet, which lend his collection a profile unmatched in Romania.