Provenance and tectonic setting of clastic rocks of the Neoproterozoic Ocoee Supergroup were assessed using modes of detrital framework minerals, detrital feldspar chemistry, whole-rock geochemistry, heavy mineral assemblages and chemistry, and detrital zircon U-Pb geochronology. Putative source rocks comprising locally exposed Grenville basement were analyzed for comparison. Samples studied are primarily arkosic to subarkosic siltstones, sandstones, and minor conglomerate. Ternary tectonic discrimination diagrams indicate a continental basement uplift setting, although the mineralogically most mature Longarm quartzite indicates a continental interior setting. The range of detrital feldspar compositions among Ocoee units is comparable to feldspar in basement rocks. Orthoclase-rich detrital alkali feldspar predominates over detrital albitic plagioclase. Whole-rock normative Qz-Or-Pl values and trace-element abundances closely match those of local basement. Snowbird Group siltstones and sandstones contain high abundances of zircon, apatite, titanite, ilmenite, and epidote, which locally occur as concentrations of heavy minerals in discrete laminae. Zircon-tourmaline-rutile indices and titanite compositions are most consistent with a granitic source for these sediments. The majority of detrital zircon U-Pb ages are late Mesoproterozoic, with scattered late Neoproterozoic and Paleoproterozoic grains. All but one of the ∼1200 detrital zircons (at ca. 2000 Ma) can be accounted for by a local Blue Ridge basement magmatic source terrane. Archean detrital zircon ages are absent from the Ocoee detrital zircon age population. This absence is consistent with the general paucity of Archean grains in other Neoproterozoic Southern Appalachian clastic sequences. All data are consistent with a lithologically and geochronologically restricted, proximal, flank source for sediment filling a marginal continental rift. The Ocoee represents the first pulse of sediment dominated by Grenville-age zircon on the eastern Laurentian margin and serves as a major source of recycled zircon for Paleozoic clastic sequences in eastern Laurentia. The youngest detrital zircon age obtained from the basal Ocoee Wading Branch Formation (639 ± 8 Ma) provides a maximum depositional age for the Ocoee Supergroup and onset of rift-filling sedimentation in the intracontinental Ocoee basin.