The museum is housed in one of Athens’ most attractive 19th century buildings, designed by Stamatis Kleanthis. The eccentric Sophie de Marbois-Lebrun, Duchess of Plaisance, lived here until her death in 1854. In 1926 the Villa Ilissia was chosen as the home of the Byzantine and Christian Museum, one of the most important museums of its kind in the world, dedicated to Byzantine and post-Byzantine art and culture.

Its collections comprise 25,000 artifacts from different parts of Greece, Asia Minor and the Balkans, organized into collections spanning the period from the 3rd century AD to the 20th century.