The Municipality of Athens began to put together its artist collection in 1923. The first work it bought was the sculpture by D. Philippotis, "The Fisherman", and it is interesting to note that half of the 2,355 works of art which the Gallery counts among its collection, were acquired during the period 1930-1940.

Almost all the Greek artists, whose creations marked the history of Greek art and who contributed to its development in the 20th century, are represented by some of their important works in the collection of the Municipal Gallery. Among its most interesting features are the collection of engravings, with works by the great masters of this art and their worthy followers, but also of works by young engravers; the full representation of the generation of artists of the '30s; the collection of works by the famous architect, Ziller, which are of artistic and historical interest, and among which are 56 drawings of the National Theatre, the Municipal Theatre, as well as of private homes; also the paintings of ruins by V. Lanza; the portraits of Mayors and Presidents of Municipal Councils painted by masters of the style (Tsokos, Kalloudis, Iakovides) and a large number of drawings of the Arts Sanctuary inspired from the Athens of their time.