The igneous protoliths of the Margaree orthogneiss intruded the peri-Gondwanan rocks of the Port-aux-Basques Complex, in the southwestern corner of the Hermitage Flexure, prior to regional deformation and metamorphism. Field relationships and U–Pb geochronology indicate that the Margaree orthogneiss represents a 20 km long, mafic–felsic intrusive complex formed by amphibolite, dioritic orthogneiss, Ma hornblende-bearing tonalitic orthogneiss with mafic enclaves, 472 ± 2.5 Ma and 465 ± 3 Ma biotite-bearing granitic orthogneiss, and minor ultramafic rocks. Most amphibolite have the chemistry of volcanic-arc tholeiite and are interpreted to be coeval with the intrusion of tonalitic and granitic magma with volcanic-arc geochemical signatures. Locally, mafic magmatism continued after the intrusion of the 465 Ma granite. The Margaree orthogneiss and its country rock were overprinted by upper amphibolite-facies metamorphism and deformation associated with the final closure of the Iapetus Ocean. A late-synkinematic granite dates the late stages of the high-temperature regional deformation at Ma, while metamorphic titanite (411 ± 2 Ma) is interpreted to date extensive recrystallization under amphibolite-facies conditions as Early Devonian. The Margaree orthogneiss is broadly coeval with the plutons that postdate the Early Ordovician Penobscottian arc – passive margin imbrication in central and southern Newfoundland. It also coincides with the extensive late Arenig – early Llanvirn back-arc rifting event along the entire peri-Gondwanan margin of the northern Appalachians. The external position of the Port-aux-Basques Complex with respect to the back-arc elements in the Hermitage Flexure, coupled with the rock types and geochemistry of the orthogneiss, suggest formation of the Margaree orthogneiss in an arc and (or) back-arc transitional setting.