It displays many of the works amassed by shipowner Basil Goulandris and his wife Elise Karadontis, who died in 1994 and 2000 respectively, with an art collection valued at US$3 billion.

It is housed in a 1920s neoclassical mansion with a ten-storey new extension (five of which are below ground).

[citation needed] The building also houses a museum shop and a café-restaurant.

[citation needed] The floors below ground hosts a library with around 4,500 books, a children's workshop, and a 190-seat amphitheatre.

[citation needed] Basil Goulandris collected works by artists including Pablo Picasso, Marc Chagall, Henri Matisse, Alberto Giacometti, Auguste Renoir, Joan Miro, Paul Klee, Wassily Kandinsky, El Greco, Cézanne and Modigliani, as well as works by Greek modern painters including Parthenis, Bouzianis, Vasileiou, Hadjikyriakos-Ghika, Tsarouchis, Moralis, and Tetsis.