Ordovician metamorphic rocks of the Casco Bay Group are exposed in an approximately 170 km long NE-trending belt (Liberty-Orrington belt) in southern and south-central Maine. Geochemical analysis of rocks within the Spring Point Formation (469 ± 3 Ma) of the Casco Bay Group indicate that it is an assemblage of metamorphosed bimodal volcanic rocks. The mafic rocks (originally basalts) have trace element and Nd isotopic characteristics consistent with derivation from a mantle source enriched by a crustal and/or subduction component. The felsic rocks (originally rhyolites and dacites) were likely generated through partial melting of continental crust in response to intrusion of the mafic magma. Relatively low initial εNd values for both the mafic (−1.3 to +0.6) and felsic (−4.1 to −3.8) rocks suggest interactions with Gander zone continental crust and support a correlation between the Casco Bay Group and the Bathurst Supergroup in the Miramichi belt of New Brunswick. This correlation suggests that elements of the Early to Middle Ordovician Tetagouche-Exploits back-arc basin can be traced well into southern Maine. A possible tectonic model for the evolution of the Casco Bay Group involves the initiation of arc volcanism in Early Ordovician time along the Gander continental margin on the eastern side of the Iapetus Ocean basin. Slab rollback and trenchward migration of arc magmatism initiated crustal thinning and rifting of the volcanic arc around 470 Ma and resulted in the eruption of the Spring Point volcanic rocks in a back-arc tectonic setting.