Neoproterozoic to Paleozoic sedimentation shows systematic temporal-spatial variations within South China, which must be considered in reconstructing geological evolution of South China in response to global plate reorganization from the breakup of Rodinia to the assembly of Gondwana. We use >1000 new U-Pb and Hf isotopic data for detrital zircons from Neoproterozoic–Cambrian strata across the western (i.e., Longmenshan) and eastern (i.e., Wuyishan) margins of South China, coupled with compiled stratigraphic and magmatic information, to constrain change in provenance through time. First-order conclusions are as follows: (1) detrital zircons from the Neoproterozoic strata of the two margins were mainly sourced from the Panxi-Hannan arc and the Jiangnan orogen, signaling a rough self-sufficient sedimentary system; (2) newly identified Cambrian molasse-like sediments in the western margin, in which abundant detrital zircons are 550–500 Ma old with positive εHf(t) values, were mainly derived from the 580–500 Ma Cadomian arc belt along the Iran-Turkey margin; and (3) the Cambrian sediments in the eastern margin document more increased contributions from the Grenvillian-age provinces most possibly in Australia. Such spatial-temporal provenance variations signal the northward drifting of South China, from a position connecting with Iran-Turkey and northern India to that approaching Australia during the late Neoproterozoic–Cambrian period. We highlight that the activity of oblique oceanic-continental convergence accreted Asian terranes onto the northern margin of Gondwana, hence contributing to the ultimate Gondwana architecture under global plate reorganization.