The Lower Devonian Sainte-Marguerite volcanic rocks are part of a Silurian–Devonian volcanic sequence deposited between the Taconian and Acadian orogenies in the Gaspé Peninsula, Quebec, Canada. The Sainte-Marguerite unit includes basaltic and dacitic lava flows with calc-alkaline and volcanic-arc affinities. Such affinities are also recorded by the trace-element signature in Lower Silurian and most Lower Devonian volcanic units of the Gaspé Peninsula. However, most of the other Silurian–Devonian volcanic rocks occurring in the Gaspé Peninsula have been previously interpreted to have erupted in an intracontinental setting. A back-arc setting for the Gaspé Peninsula between the Taconian and Acadian orogenies could account for these subduction volcanic-arc signatures, though a metasomatized lithospheric mantle magma source, unrelated to subduction, cannot be excluded. Lower Silurian and Lower Devonian volcanic rocks in the central part of the Gaspé Peninsula show an arc affinity, whereas Upper Silurian and Lower to Middle Devonian volcanic rocks, located in the south and north of the Gaspé Peninsula, respectively, show a within-plate affinity. The Lower Devonian Archibald Settlement and Boutet volcanic rocks of the southern and northern Gaspé Peninsula, respectively, show a trend toward a within-plate affinity. This suggests that within-plate volcanism migrated from south to north through time in an evolving back-arc environment and that the subduction signature of Lower Silurian and Lower Devonian rocks results from a source that melted only under the central part of the Gaspé Peninsula.