Nd isotopic data from 18 felsic plutonic and volcanic units in Cape Breton Island show variations consistent with other geological and geophysical evidence for at least three distinct terranes. A ca. 1.2 Ga syenite considered to be part of Grenvilleage basement exposed in the northwestern part of the island yields an initial εNd value of +0.4 and a depleted-mantle model age (TDM) of 1.66 Ga, suggesting substantial involvement of older (Archean or Early Proterozoic) crust in its petrogenesis. A TDM of 1.38 Ga indicated by Nd isotopic data for a Devonian granite spatially associated with the syenite is also consistent with the presence of older crust in that part of Cape Breton Island. In contrast, Silurian rhyolite and Devonian granites from the Aspy terrane have TDM ranging from 0.7 to 1.1 Ga and initial εNd between +2.8 and −1.2, and overlap in isotopic characteristics with late Precambrian and Early Ordovician plutons in the Bras d'Or terrane that yield TDM of 0.9–1.1 Ga and initial εNd of +1.4 to −1.8. The relatively small variation in εNd and TDM in these terranes suggests that old crust like that under the Blair River Complex may not be present. Granitic plutons and rhyolite in the Mira terrane of southeastern Cape Breton Island have a range in TDM (0.8–1.2 Ga) similar to that of the Aspy and Bras d'Or terranes, but initial εNd values ranging from +0.8 to +5.0 indicate more juvenile crust. This juvenile crust also appears to be present under southern New Brunswick and eastern Newfoundland and may be characteristic of the Avalon terrane.