The care for the creation of artistic collections is almost contemporaneous with the independent Greek state and expresses the desire of the Greeks to see a renaissance of the arts in what has been their ancient cradle. In 1836, the famous Bavarian architect Leo von Klenze draws a magnificent plan, proposing a "Pantechnion," aspiring to host not only the archaeological collections and the School of Arts, but also an Art Gallery. This imposing hall of the arts was never to materialize. In 1878, the first nucleus of the Gallery, comprising 117 works by Greek and European artists, mainly envisaged as an educational annex to the School of Arts, was established in the Technical University of Athens and opened for the public.

In 1896, Alexandros Soutsos, a jurist and art lover, bequeathed his collection and estate to the Greek State aspiring to the creation of a “Museum of Fine Arts”. The National Gallery eventually came into being by an April 10, 1900 decree and an invitation to the painter Georgios Iakovidis to return from Munich. He became its curator in July 28, 1900. Originally in the Technical University and the University collections, a total of 258 works were donated to the newly established Gallery; the 107 works donated by Alexandros Soutsos followed suit in 1901.