Fieldwork coupled with U–Pb dating has clarified the relationships between the Exploits and Gander-derived rocks in central Newfoundland during the Mid-Ordovician opening of the Exploits back-arc basin, reinforcing correlation across the peri-Gondwanan segments of the Appalachian–Caledonian orogen. We have separated a new back-arc-related unit, the Red Cross Group, from the arc-related Victoria Lake Supergroup. This group includes 466 ± 3 Ma felsic volcanic rock interlayered with alkali basalt–enriched mid-ocean ridge basalt, 457 ± 6 Ma gabbro, Llanvirn–Caradoc normal mid-ocean ridge basalt–island arc tholeite, limestone, black shale and mélange. Locally the Red Cross Group is in parautochthonous contact with low-grade Gander psammite. This contact was overrun by the Meelpaeg Metamorphic Nappe during the Devonian. The nappe contains Gander metapsammite (Meelpaeg Subzone) and the coticule-bearing Howley Waters Complex (Exploits), which hosts 467 ± 3 Ma felsic porphyry. The Gander and Exploits metasediments in the nappe are stitched by Arenig–Llanvirn granite (467 ± 6 Ma and 468 +3.5/−3 Ma) and Caradoc intrusions (458 ± 3 Ma and 454 ± 2 Ma). Metamorphic monazite (462 ± 1 Ma) and titanite (460 ± 3 Ma) from the nearby Mount Cormack Subzone (Gander) indicate the coeval formation of a low-pressure–high-temperature metamorphic dome. The widespread presence of Caradoc magmatism suggests that the width of the back-arc basin remained relatively narrow.