Detrital muscovite from lowermost Cambrian sequences exposed in the Avalon Composite Terrane in Nova Scotia and New Brunswick record 40Ar/39Ar plateau ages of ca. 625–600 Ma. These are interpreted to date times of cooling in source areas. The regional distribution of coarse-grained detrital muscovite in Lower Cambrian rocks of Avalonian overstep sequences suggests a source region of dimensions considerably larger than any presently exposed in Appalachian segments of the Avalon Composite Terrane. Late Proterozoic tectonic reconstructions locate the Avalon Composite Terrane adjacent to northwestern South America, thereby suggesting a possible source within Late Proterozoic PanAfrican – Brasiliano orogens. Detrital muscovite from clastic sequences of the proximally derived, Lower Carboniferous (Tournaisian) Horton Group and the more distal Upper Carboniferous (Westphalian D – Stephanian) Pictou Group in Nova Scotia records 40Ar/39Ar spectra that define plateau ages of ca. 390–380 Ma (Horton Group) and and ca. 370 Ma (Pictou Group). Finer grained fractions from samples of the Horton Group display more internally discordant age spectra defining total-gas ages of ca. 397–395 Ma. A provenance for the finer muscovite may be found in southern Nova Scotia where Cambrian–Ordovician turbidites of the Meguma Group display a regionally developed micaceous cleavage of this age. The ca. 390–380 Ma detrital muscovites probably were derived from granite stocks presently exposed in proximal areas of northernmost Cape Breton Island. A more distal source for the ca. 370 Ma detrital muscovites in the Pictou Group is suggested by its original extensive distribution, although a local, possibly recycled, source may also have been present. The presence of only 400–370 Ma detrital muscovite suggests a rapidly exhumed orogenic source with characteristics similar to those of crystalline rocks presently exposed in the Cape Breton Highlands and (or) the Meguma Terrane.