Fifteen U–Pb (zircon) radiometric age determinations have been made on igneous rocks of Middle Devonian to Early Carboniferous age from the southern margin of the Magdalen basin in Cape Breton Island and northern mainland Nova Scotia. Volcanic rocks interbed with early rift-basin sedimentary rocks with some palynological biostratigraphy; dated intrusive rocks cut these sedimentary units. Our biostratigraphically constrained ages are in close agreement with the current Devonian time scale. Combined with previously published data, the age determinations show that igneous activity occurred in four pulses: Middle Devonian (390–385 Ma), early Late Devonian (375–370 Ma), latest Devonian to early Tournaisian (365–354 Ma), and late Tournaisian to early Visean (ca. 339 Ma). Middle Devonian (385–389 Ma) volcanic rocks are confined to the Guysborough Group. The Fisset Brook Formation (basalt and minor rhyolite) in the type area and elsewhere in Cape Breton Island and northern mainland Nova Scotia is Late Devonian (ca. 373 Ma), whereas the biostratigraphically distinct succession at Lowland Cove is younger (365 Ma). These Late Devonian rocks are synchronous with plutonism in the Cape Breton Highlands and the Meguma terrane. In the Cobequid Highlands, rhyolite of the Fountain Lake Group was synchronous with Horton Group deposition and with widespread granite plutons (362–358 Ma) emplaced during shear on the Cobequid fault zone. The overlying Diamond Brook Formation basalts are slightly younger (355 Ma). Late Tournaisian – early Visean mafic intrusions and minor basalt occur along the Cobequid – Chedabucto fault zone and in a belt from southern New Brunswick through Prince Edward Island to southwestern Cape Breton Island.