The Yarmouth Island Formation of the East Harpswell Group (EHG) is an assemblage of metamorphosed volcanic and sedimentary rocks exposed in Casco Bay, Maine. Although previously interpreted to have been deposited ca. 445 Ma, two new U–Pb zircon ages from metavolcanic rocks in the unit indicate prolonged magmatism between ca. 469–474 Ma and correlation with adjacent rocks of the more regionally extensive Casco Bay Group (CBG) in the Liberty–Orrington belt. New detrital zircon results from metasedimentary rocks in the EHG support this correlation; the age spectra indicate a peri-Gondwanan sedimentary source, consistent with earlier published results from the CBG. Detailed geochemical studies of the metavolcanic rocks in the Yarmouth Island Formation indicate a wide range of sub-alkaline compositions (SiO2 = 47.9–77.5 wt.%), flat chondrite-normalized rare earth element distributions, and a prominent negative Nb anomaly in normalized spider plots. Tectonic discrimination plots suggest eruption in a volcanic arc setting with continental crustal influence. This tectonic setting, when combined with the co-existence of marine sedimentary rocks, suggests a transitional setting between that of subduction and subsidence in a marine setting, perhaps due to the onset of back-arc rifting. Similarities in age, lithologic character, sediment provenance, and volcanic rock geochemistry indicate a strong correlation between these rocks in the Liberty–Orrington belt and those along strike in the southern portion of the Miramichi belt of eastern Maine and southern New Brunswick. These findings confirm the preservation of >500 km long, ca. 470 Ma, arc/back-arc terrane within the Ganderia superterrane in the northern Appalachians.