A holoplanktonic mollusc assemblage from Neogene sediments of the Azorean island Santa Maria is described and analysed to determine the age of the sediments. Sixteen taxa are documented (three heteropods, thirteen pteropods), fourteen of which are new records for the fossil fauna of Santa Maria Island. The composition of the heteropod and pteropod assemblage indicates a Zanclean age, which contrasts with earlier age assignments to the Early, Middle or Late Miocene based on benthic molluscs, but is in good agreement with more recent data based on foraminiferal and geochemical evidence. The pteropod Cavolinia marginata (BRONN, 1862) is re-described based on abundant topotypic material and a neotype is designated. The species Cavolinia vendryesiana (GUPPY, 1873) is considered to be a junior subjective synonym of C. marginata. The temporal range of the pteropod Limacina trochiformis (D.ORBIGNY, 1836) is extended to the Zanclean.