The southern Appalachian crystalline core is composed of lithotectonic assemblages that are largely sedimentary in origin. Sixteen paragneiss samples from the Blue Ridge and Inner Piedmont of North Carolina and Georgia, and one sample of Middle Ordovician rocks from the Sevier-Blountian clastic wedge in the Tennessee Valley and Ridge were sampled for sensitive high-resolution ion microprobe (SHRIMP) U-Pb detrital zircon geochronology, whole-rock geochemistry, and zircon trace-element analyses. Detrital zircon ages range from Archean (~2.7 Ga) to Middle Paleozoic (~430 Ma), with a notable abundance of Mesoproterozoic zircons (1.3–0.9 Ga). Many samples also contain moderate populations of slightly older Mesoproterozoic zircons (1.5–1.3 Ga). Minor populations of Paleoproterozoic (2.3–1.5 Ga) and Neoproterozoic (754–717 and 629–614 Ma) ages occur in several samples; however, Paleozoic detrital zircons (478–435 Ma) are restricted to samples from the Cat Square terrane. Depositional periods of the metasedimentary terranes are bracketed by detrital zircon, metamorphic, and magmatic ages, and include: (1) Mesoproterozoic, (2) Neoproterozoic to early Paleozoic, and (3) middle Paleozoic. A xenolith from the ~1.15 Ga Wiley Gneiss suggests a post–~1.2 Ga period of sedimentation prior to the ~1.15 Ga Grenvillian magmatic event. Detrital zircon populations of Neoproterozoic to Middle Ordovician suggest a mixed Laurentian provenance with Amazonian and peri-Gondwanan sources deposited in divergent and convergent plate settings. Blue Ridge and Inner Piedmont detrital zircon ages, whole-rock geochemistry, lithologic assemblages, and field relationships are compatible with deposition of immature clastic material in a rift and passive-margin setting from the Neoproterozoic to early Paleozoic. Occurrence of 1.3–0.9 Ga, 1.5–1.3 Ga, and 754–717 Ma detrital zircon ages indicate a dominantly Laurentian provenance for the Cartoogechaye, Cowrock, Dahlonega gold belt, Smith River allochthon, and Tugaloo terranes. Minor Paleoproterozoic populations in these terranes suggest input from distal terranes of the Laurentian midcontinent or the Amazonian craton. Transition to a convergent plate margin in the Middle Ordovician resulted in collision of central Blue Ridge and Tugaloo terranes and recycling of material from these terranes into the Mineral Bluff Formation and Sevier Shale. Ordovician and 629–614 Ma detrital zircons from the Cat Square terrane document the first occurrence of peri-Gondwanan material, which was deposited in a convergent setting between the Laurentian margin and the accreting Carolina superterrane during the Late Silurian to Devonian.