Interlayered mafic and felsic metavolcanic rocks and metasedimentary rocks of Ordovician to Silurian age are characteristic of the Aspy terrane of northwestern Cape Breton Island. These rocks were affected by medium- to high-grade metamorphism and were intruded by synkinematic granitoid orthogneisses during Late Silurian to Early Devonian times. They were intruded by posttectonic Devonian granitic plutons and experienced rapid Devonian decompression and cooling. The chemical characteristics of the mafic metavolcanic rocks indicate that they are tholeiites formed in a volcanic-arc setting. The volcanic rocks of the Aspy terrane differ from many other Silurian and Silurian–Devonian successions in Atlantic Canada, which have chemical and stratigraphic characteristics of volcanic rocks formed in extensional within-plate settings, and are somewhat younger than the Aspy terrane sequences. Aspy terrane units are most similar to Ordovician–Silurian volcanic and metamorphic units in southwestern Newfoundland, including the La Poile Group and the Port aux Basques gneiss. Together with other occurrences of Late Ordovician to Early Silurian volcanic-arc units, they indicate that subduction-related compressional tectonics continued into the Silurian in parts of the northern Appalachian Orogen. The complex Late Silurian – Devonian tectonic history of the Aspy terrane may reflect collision with the southeastern edge of a Grenvillian crustal promentory.