Sculpture also features prominently, both in terms of the variety of types (crucifixes, rondes-bosses, bas-reliefs) and iconography: statues of saints and crucifixes from the 16th and 17th centuries - including a Virgin carved in wood by Pasquier Borreman - stand alongside 19th-century royal bust portraits and commemorative plaques of doctors who worked in institutions attached to the CPAS in the City of Brussels.

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Among the most remarkable pieces are a 14th-century head of a man attributed to the sculptor Claus Sluter, a bronze by the celebrated Romantic artist Antoine-Louis Barye, and a large series of rondes-bosses by Émile Namur.