ABSTRACT The timing and kinematics of Paleozoic peri-Gondwanan terrane accretion along the southern and central Appalachian margin have long been debated. The Silurian–Devonian Concord plutonic suite intruded the western flank of the Carolina superterrane, suggesting east-dipping subduction of ocean crust beneath the Carolina superterrane just prior to accretion, based on Devonian–Mississippian plutonism and metamorphism in the adjacent Laurentian terranes. Geochemical and isotopic data support a subduction-related origin for the Concord plutonic suite, and our geochronologic data reveal the main pulse of plutonism occurred ca. 405 Ma. Our new sensitive high-resolution ion microprobe (SHRIMP) geochronologic data identify a suite of mafic plutons from the Carolinas to central Georgia that also belong to the Concord suite. These gabbros have U-Pb zircon ages of 372 ± 2 Ma (Gladesville contact aureole), 386 ± 5.7 Ma (Buffalo), 403.8 ± 3.7 Ma (Highway 200), 404.9 ± 6.9 Ma (Mecklenburg), and 416 ± 6.9 Ma (Calhoun Falls). The Ogden Gabbro has a U-Pb age from baddeleyite of 411.91 ± 0.25 Ma. In this study, we identified a previously unrecognized Alleghanian (Pennsylvanian) gabbro suite with U-Pb zircon ages of 308.2 ± 6.2 Ma (Farmington), 311 ± 6.2 Ma (Dutchman’s Creek), and 311 ± 6.5 Ma (Mount Carmel). These gabbros should henceforth not be included in the Concord suite. The ages of Concord suite plutons slightly predate the main phase of plutonism in the Cat Square terrane to the west, which we suggest represents the product of B-type subduction of ocean crust beneath the Carolina superterrane between 415 and 400 Ma. Arc-related magmatism terminated because of the switch to A-type subduction of the eastern Laurentian margin. Prograde upper-amphibolite- to granulite-facies metamorphism, wholesale migmatization, and extensive anatectic plutonism in the eastern Inner Piedmont occurred from Late Devonian into Mississippian time, shortly after cessation of Concord plutonic suite plutonism, which also supports this proposed model. These data, combined with the timing and geometry of foreland clastic wedges, provide compelling support for Devonian–Mississippian accretion of the Carolina superterrane via dextral transpressive obduction above the eastern Laurentian margin.