The Fisset Brook Formation of western Cape Breton Island and its equivalents at MacMillan Mountain and the north Baddeck River are examples of Late Devonian and Early Carboniferous volcanic sequences associated with the formation of post-Acadian successor basins in the northeastern Appalachians. They consist of bimodal basalt–rhyolite suites interbedded with alluvial fan, lacustrine, and rare fluvial sediments. The earliest volcanic products are rhyolites and somewhat evolved basalts associated with coarse sediments, followed by tholeiitic to transitional basalt flows interlayered with lacustrine-type deposits. Geochemical studies on the Fisset Brook Formation indicate extensive remobilization of alkalies, Ca, Rb, and Sr, making these elements inappropriate for determining tectonic setting or magmatic affinity. Use of less mobile elements (Ti, Nb, Y, and Zr) suggests that the basalts are tholeiitic and that the apparent alkalinity of the type section lavas is a result of alteration. We conclude that volcanism in western Cape Breton Island started at MacMillan Mountain and migrated westwards, probably towards the centre of the deepening Magdalen Basin.