The Museum has a very large collection of sculpture (ca 2,000 pieces).  At its heart are the sculptures dated to the Byzantine period (324-1453).  The majority of them are architectural members, which were collected over time from various monuments and sites in Athens.  To these have been added sculptures from the rest of Greece, including the Peloponnese, Thessaloniki, Nea Anchialos (formerly Phthiotic Thebes), as well as Asia Minor.  The sculpture in the collection gives a historical overview of Byzantine sculpture, above all that of Southern Greece.  Thus we find works attributed to the fifth and sixth centuries, that is the period of the great building programmes of the new religion; from the period between the seventh and ninth centuries, when the world of Late Antiquity was transformed into the Middle Ages; and finally the later centuries, which saw exceptional building activity in Southern Greece, in which sculpture plays a striking role from both a quantitative and qualitative point of view. The Byzantine period ends with the "Franco-Byzantine" works, artistic testimonies to the new historical circumstances in the Aegean after the Fourth Crusade of 1204 and before the fall of Byzantium in 1453.  As regards the years after the Fall, the Byzantine Museum's Collection includes sculptures from both Moslem and Christian monuments in Athens, works from the islands under the sphere of influence of Venice and Genoa (i.e. Crete, the Ionian Islands and Chios) as well as from the Cyclades, above all Tinos, the sculpture production of which leads us to the academicizing Modern Greek sculpture of the nineteenth century.
   
In addition to the above the Museum's collection includes a body of Roman architectural sculpture, table supports, a female portrait bust and fragments of sarcophagi.  The group of Coptic architectural and funerary reliefs, which represent sculpture produced in Egypt in the Late Antique period, is an important part of the collection. Finally it should be noted that some funerary and masonry inscriptions from Athens carved on stone slabs belong in the Byzantine section, as do two notable relief icons of the Virgin from Thessaloniki.
   
The Museum's main aim is, on the one hand, to systematically document and publish its extensive, though sometimes problematic, material using the approaches offered by modern research and on the other to expand the collection with new acquisitions, so as to present a balanced historical overview of sculpture from the Roman period up to modern times.