Mount Etna lies near the boundary between two regions that exhibit significantly different types of volcanism. To the north, volcanism in the Aeolian island arc is thought to be related to subduction of the Ionian lithosphere. On Sicily itself, however, no chemical or seismological evidence of subduction-related volcanism exists, and so it is thought that the volcanism-including that on Mount Etna itself-stems from the upwelling of mantle material, associated with various surface tectonic processes. But the paucity of geological evidence regarding the primary composition of magma from Mount Etna means that its source characteristics remain controversial. Here we characterize the trace-element composition of a series of lavas emitted by Mount Etna over the past 500 kyr and preserved as melt inclusions inside olivine phenocrysts. We show that the compositional change in primary magmas from Mount Etna reflects a progressive transition from a predominantly mantle-plume source to one with a greater contribution from island-arc (subduction-related) basalts. We suggest that this is associated with southward migration of the Ionian slab, which is becoming juxtaposed with a mantle plume beneath Sicily. This implies that the volcanism of Mount Etna has become more calc-alkaline, and hence more explosive, during its evolution.