Amygdaloidal basaltic flows of the Ashfield Formation were encountered in two drill holes in areas of positive aeromagnetic anomalies in the Carboniferous River Denys Basin in southwestern Cape Breton Island, Nova Scotia. One sample of medium-grained basalt yielded a plateau age of 201.8 ± 2.0 Ma, similar to the U–Pb and 40Ar/39Ar crystallization ages from basaltic flows and dykes in the Newark Supergroup. A second sample of zeolite-bearing basalt yielded a discordant age spectrum and a younger age of ca. 190 Ma, which is interpreted to date a widespread hydrothermal event related to zeolite formation. Whole-rock chemical data show that the Ashfield Formation basalt is low-Ti continental tholeiite, consistent with its within-plate tectonic setting. Chemically, it resembles basaltic flows in the Mesozoic Fundy and Grand Manan basins exposed in southern Nova Scotia and eastern New Brunswick and elsewhere in Central Atlantic Magmatic Province (CAMP). The age and geochemical data from the Ashfield Formation provide the first evidence for early Mesozoic CAMP volcanism in Cape Breton Island and demonstrate that the event was more widespread in Nova Scotia than previously thought, which has implications for its continuity and extent elsewhere within CAMP.