Avalonia is a terrane that accreted to Laurentia–Baltica during the development of the Appalachian–Caledonide Orogen. Interpretations of the timing of accretion have been constrained by comparing faunal affinities, overstep sequences, age and kinematics of inferred accretionary deformational events, and controversial paleomagnetic data. We show that the time of accretion of Avalonia may also be constrained by contrasts in the geochemical and isotopic signatures of its igneous rocks (which reflect the characteristics of the underlying continental basement and mantle) and sedimentary rocks (which reflect provenance). Early Silurian clastic sedimentary rocks of the Beechill Cove Formation, Antigonish Highlands, Nova Scotia, were deposited on Avalonian crust. The formation predominantly consists of approximately 80 m of siltstones and shales deposited in a nearshore environment and derived from the northeast. Their age is constrained by paleontological data and by directly underlying Late Ordovician – Early Silurian bimodal volcanic rocks that have typically Avalonian geochemical signatures. In comparison with typical Avalonian rocks, the Beechill Cove sediments are characterized by high SiO2, Ce/Yb, and initial 87Sr/86Sr, low Fe2O3, MgO, and TiO2, and strongly negative εNd(ur). These characteristics cannot be attributed to erosion of underlying Avalonian basement or coeval volcanic rocks and are consistent with derivation via significant transport from radiogenically enriched continental crust. εNd data are typical of Grenvillian basement compositions and suggest that the Beechill Cove sedimentary rocks were derived from an adjacent landmass with Grenvillian crust. The data, in conjunction with paleocontinental reconstructions and recent geochronological and structural data from the northern Appalachians, suggest that the Caledonide orogenic belt is the most likely source. Deposition of the Beechill Cove Formation is inferred to have occurred in an intracontinental basin associated with strike-slip tectonics during the oblique collision of the Avalon with Laurentia–Baltica.