New geologic mapping coupled with uranium-lead (U-Pb) zircon geochronology (sensitive high-resolution ion microprobe-reverse geometry [SHRIMP-RG] and laser ablation-inductively coupled plasma-mass spectrometry [LA-ICP-MS]) analyses of 10 samples, provides new constraints on the tectonostratigraphic framework of the central Virginia Piedmont. Detrital zircon analysis confirms that the Silurian-Devonian Quantico Formation is a postorogenic successor basin, with zircons derived primarily from Ordovician Chopawamsic Formation volcanic rocks. Detrital zircons from strata of the Long Island syncline, previously mapped as a separate successor basin, have a peri-Gondwanan component distinct from Laurentian-sourced rocks of the Potomac terrane to the west. Volcanism of the Chopawamsic Formation spanned at least 14 million years during the Ordovician. The Chopawamsic Formation contains sheet-like Late Ordovician-Silurian granodioritic and tonalitic intrusions that were once mapped as Carboniferous. Biotite-muscovite migmatitic paragneiss, which borders the Chopawamsic Formation on its southeast side and also occurs east of the Lakeside fault, preserves evidence of Silurian deformation and metamorphism, with a Carboniferous (Alleghanian) overprint. Limited SHRIMP-RG analysis of detrital zircons from this paragneiss yields a Laurentian (Mesoproterozoic) signature, which suggests that the structurally concordant contact between volcanic rocks of the Chopawamsic Formation and paragneiss is either a pre-Alleghanian fault or an unconformity.