To better understand the evolution of the South China Craton (SCC), we have determined the geochronological and geochemical compositions of newly recognized Grenville-aged metabasalts in the Shennongjia region of the northern Yangtze block. LA-ICP-MS U-Pb dating of zircons indicates that the metabasalts formed at 1063 ± 16 Ma. The rocks are calc-alkaline, are characterized by SiO2 contents (50.50 to 55.62 wt.%), and have moderate-to-high MgO contents (7.25–9.60 wt.%). They display light rare earth element enrichment ((La/Yb)N = 7.0–9.8) with slightly negative Eu anomalies (Eu/Eu* = 0.82–0.90) and have pronounced depletion in high-field strength elements as well as positive Pb anomalies in the primitive mantle-normalized trace element pattern. They possess high initial Sr isotopic ratios of 0.7092–0.7107, large negative εNd(t) values of −12.1 to −11.0, and a relatively narrow range of initial Pb isotope ratios (206Pb/204Pb = 16.503–17.019, 207Pb/204Pb = 15.259–15.452, and 208Pb/204Pb = 36.169–36.994). These isotopic characteristics are typical of basalts derived from an EM2 source region and suggest a subcontinental lithospheric mantle source that was metasomatized by subducted components (fluids and melts). Integrating our new data with documented igneous and metamorphic events during late Mesoproterozoic to early Neoproterozoic time in the region and western segments of the Yangtze block, we suggest that the Shennongjia area might be a microcontinent that was independent of the continental nucleus of the Yangtze block and was accreted to the Yangtze block at the end of Mesoproterozoic time. This study thus argues against the traditional view that the SCC was formed simply by Yangtze–Cathaysia collision and supports a hypothesis in which the Yangtze block was a collage of microcontinents accreted during the Grenvillian period accompanying the assembly of the Rodinia supercontinent.