The Walker Top Granite (here formally named) is a peraluminous megacrystic granite that occurs in the Cat Square terrane, Inner Piedmont, part of the southern Appalachian Acadian-Neoacadian deformational and metamorphic core. The granite occurs as disconnected concordant to semi-concordant plutons in migmatitic, sillimanite zone rocks of the Brindle Creek thrust sheet. Locally garnet-bearing, the Walker Top Granite contains blocky alkali feldspar megacrysts 1–10 cm long in a groundmass of muscovite-biotite-quartz-plagioclase-alkali feldspar and accessory to trace zircon, titanite, epidote, sillimanite (xenocrysts), and apatite. It varies from granite to granodiorite and contains several xenoliths of biotite gneiss, amphibolite, quartzite, and in one location encloses charnockite (here formally named Vale Charnockite). New sensitive high-resolution ion microprobe U-Pb zircon magmatic crystallization ages obtained from the plutons of the Walker Top Granite are: 407 ± 1 Ma in the Brushy Mountains; 366 ± 2 Ma in the South Mountains; and 358 ± 5 Ma in the Vale–Cat Square area. An age of 366 ± 3 Ma was obtained from the Vale Charnockite at its type locality. Major-, trace-element, and isotopic chemistry indicates that Walker Top is a high-K, peraluminous granite, plotting as volcanic arc or syn-collisional on tectonic discrimination diagrams and suggests that it represents deep-seated anatectic magma with S- to I-type affinity. The alkali calcic, ferroan Vale Charnockite likely formed by deep crustal melting, and similar geochemical and trace-element compositions suggest a similar tectonic origin as Walker Top Granite. The discontinuous nature of the Walker Top Granite plutons precludes it intruded as a volcanic arc. Instead, the peraluminous nature, common xenoliths of surrounding country rock, and geochemical and isotopic signatures suggest it formed by partial melting of Cat Square and Tugaloo terrane rocks. Following emplacement and crystallization, Walker Top plutons were deformed into elliptical to linear shapes—SW-directed sheath folds—enveloped by partially melted, pelitic and quart-zofeldspathic rocks. Collectively, Walker Top and other plutons helped weaken the crust and facilitate lateral crustal flow in a SW-directed, tectonically driven orogenic channel during the Acadian-Neoacadian event. A comparison with the northern Appalachians recognizes a similar temporal magmatic and deformational history during the Acadian and Neoacadian orogenies, although while the Walker Top Granite intruded the lower plate during eastward subduction beneath the peri-Gondwanan Carolina superterrane, the northern Appalachian plutons intruded the upper plate during subduction of the Avalon superterrane westward beneath Laurentia. We hypothesize that a transform fault, located near the southern end of the New York promontory, accommodated oppositely directed lateral plate motion and different subduction polarity between the Carolina and Avalon superterranes during the Acadian and Neoacadian orogenies.