The geodynamic framework of the South China Craton in the Early Paleozoic and Early Mesozoic has been modeled as developing through either oceanic convergence or intracontinental settings. On the basis of an integrated structural, geochemical, zircon U-Pb and Hf isotopic, and mica 40Ar/39Ar geochronologic study we establish that an intracontinental setting is currently the best fit for the available data. Our results suggest that widespread tectonomagmatic activity involving granite emplacement and mylonitic deformation occurred during two distinct stages: ~435–415 Ma and ~230–210 Ma. The coeval nature of emplacement of the plutons and their ductile deformation is corroborated by the subparallel orientation of the mylonitic foliation along the pluton margins, gneissose foliation in the middle part of pluton, the magmatic foliation within the plutons, and the schistosity in the surrounding metamorphosed country rocks. The 435–415 Ma granitoids exhibit peraluminous, high-K characteristics, and zircons show negative eHf(t) values (average −6.2, n = 66), and Paleoproterozoic two-stage model ages of circa 2.21–1.64 Ga (average 1.84 Ga). The data suggest that the Early Paleozoic plutons were derived from the partial melting of the Paleoproterozoic basement of the Cathaysia Block. The 230–210 Ma granites are potassic and have zircons with eHf(t) values of −2.8–−8.7 (average −5.4, n = 62), corresponding to TDM2 ages ranging from 2.0 to 1.44 Ga (average 1.64 Ga), suggesting that the Early Mesozoic partial melts in Cathaysia were also derived from basement. The geochemical distinction between the two phases of granites traces continental crustal evolution with time, with the Early Mesozoic crust enriched in potassium, silicon, and aluminum, but deficient in calcium, relative to the Paleozoic crust. Kinematical investigations provide evidence for an early-stage ductile deformation with a doubly vergent thrusting pattern dated at 433 ± 1 to 428 ± 1 Ma (40Ar/39Ar furnace step-heating pseudoplateau ages obtained on muscovite and biotite from mylonite and deformed granite) and a late-stage strike-slip movement with sinistral sense of ductile shearing at 232 ± 1 to 234 ± 1 Ma (40Ar/39Ar furnace step-heating pseudoplateau ages) along an E-W direction. The geological, geochemical, and isotopic signatures likely reflect far-field effects in response to continental assembly events at these times.