The South China Craton consists of the Yangtze and Cathaysia blocks that were welded together along the Jiangnan Fold Belt in the Neoproterozoic. The Neoproterozoic magmatism in the western and northern margins of the Yangtze Block is characterized by voluminous volcano-sedimentary strata, numerous felsic intrusions and many mafic-ultramafic plutons which provide a good opportunity to examine the geodynamics and tectonic evolution of the South China Craton during the assembly and breakup of Rodinia. Based on the geochronological and geochemical data, our study shows that the Neoproterozoic igneous rocks in the western and northern margins of the Yangtze Block were formed in subduction- and rift-related tectonic settings, respectively. In the western margin of the Yangtze Block, the Neoproterozoic mafic and ultramafic rocks show arc-affinity trace elemental compositions that are indicative of mantle sources enriched by slab fluids. High-δ18O mafic rocks (850–780 Ma) were derived from mantle wedges that were modified by sediment melts, whereas low-δ18O mafic rocks (750–740 Ma) were formed by partial melting of mantle sources further enriched by altered oceanic crust melts. The widespread calc-alkaline I-type granitoids in this region, generated between 870 and 750 Ma, show negative to positive whole rock εNd (−4.9 to +4.8) and variable zircon εHf values (−1.9 to +10.6), similar to those of the contemporary mafic-ultramafic rocks, suggesting that they were produced by melting of the juvenile crust. The 780–750 Ma adakitic granitoids are characterized by high Sr/Y (19–318) and low Y (1.78–17.9 ppm) and have relatively constant εNd (−2.1 to +2.9) and εHf (+4.3 to +7.1) and mantle-like δ18O values (3.40‰ to 6.86‰), suggesting that they were partial melts of a subducted oceanic slab. These three types of igneous rocks demonstrate that the Neoproterozoic magmatism in the western margin of the Yangtze Block was controlled by a continuous subduction system. However, Neoproterozoic magmatism in the South Qinling Belt at the northern margin of the Yangtze Block generated both arc- and rift-related igneous rocks. The arc-like mafic-ultramafic rocks are thought to have been derived from a subduction-modified lithospheric mantle source, whereas the MORB-affinity mafic rocks were probably sourced from an asthenosphere mantle. Associated Neoproterozoic granitoids were produced by melting of the juvenile mafic crust, except minor felsic rocks derived from the ancient basement. Widespread 800–700 Ma volcano-sedimentary sequences and 650 Ma mafic dike swarms suggest an extensional environment. Neoproterozoic magmatic zircons from felsic volcanic rocks and HP/UHP metamorphic rocks preserve low-δ18O values that were inherited from their protolith which underwent high temperature hydrothermal interaction in a rift setting. On the basis of these observations, the Neoproterozoic magmatism in the South Qinling Belt is proposed to have been controlled by a subduction-transform edge propagator (STEP) in relation to the continuous subduction system at the western margin of the Yangtze Block.