New sedimentological, geochemical, and geochronological data from the Cottrells Cove Group in central Newfoundland provide important constraints on the nature of the Notre Dame Subzone, its tectonic setting, and the history of the Laurentian margin during the Early Ordovician. The Cottrells Cove Group forms the eastern extension of the Roberts Arm Group and correlates with the Chanceport Group on New World Island. It is represented by two volcano-sedimentary formations that occur in a complex thrust stack. The Fortune Harbour Formation consists of calc-alkalic, island-arc lavas, followed by a 1250 m thick succession of volcaniclastic deposits, radiolarian cherts, and calc-alkalic, mafic flows, which were deposited in a back-arc, basin-plain setting. The volcaniclastic deposits include felsic tuff, which has a U–Pb zircon age of 484 ± 2 Ma and an inheritance component of 2517 ± 26 Ma. These new U–Pb and Nd-isotope data suggest that the island-arc–back-arc volcanism and sedimentation in the Notre Dame Subzone developed in the vicinity of continental margin and approximately 10 Ma earlier than has previously been established. The Moores Cove Formation is undated but contains boulders of calc-alkalic basalt and is presumed to be at least in part younger than the Fortune Harbour Formation. Tholeiitic lavas, together with associated radiolarian cherts and volcaniclastic deposits, constitute the basal part of the Moores Cove Formation and may have been deposited in a back-arc environment synchronously with some parts of the Fortune Harbour Formation. They are conformably followed by an over 1200 m thick, coarsening-upward succession of lower-slope and submarine-fan deposits. The polymictic flysch, containing clasts of island-arc basalt, accompanied by other volcanic, plutonic, ultramafic, and sedimentary detritus, may record Middle or Upper Ordovician uplift and erosion of obducted arc–back-arc, volcano-sedimentary sequences and their ophiolitic substrate.