The Neoproterozoic mafic intrusions in the Bikou Terrane along the northwestern margin of the Yangtze Block record crucial information on evaluating the tectonic evolution of the Yangtze Block, South China. However, their petrogenesis and tectonic significance are still poorly constrained. In this paper, we present the results of a comprehensive study of zircon U–Pb geochronology and whole-rock geochemistry from the gabbro-diorites and gabbros of the Bikou Terrane. Zircon U–Pb dating results indicate that these gabbro-diorite and gabbro samples were formed coevally at ca. 880 Ma. The gabbro-diorite samples are calc-alkaline in composition and have intermediate contents of SiO2, Mg#, Ni, and Cr. They are enriched in LREEs, and depleted in HFSEs (i.e., Nb, Ta, Zr, and Hf). They have relatively high ratios of Th/Yb, and low ratios of Nb/Yb, Nb/La, Th/Nd, Th/Zr, and U/Th, indicating that they were derived from partial melting of a mantle wedge source metasomatized by slab-derived melts. The gabbro samples are commonly classified as sub-alkaline tholeiitic rocks, and have constantly low to medium values of MgO, Mg#, Cr, and Ni, with distinct spikes at Th, U, Nb and Ta concentrations. They show an E-MORB-like enriched LREEs, low ratios of Nb/La, Ta/Yb, Th/La, and Nb/Zr, and medium ratios of Nb/Yb and Th/Yb, implying that they were most probably originated from the interaction between the upwelling enriched asthenospheric mantle and the mantle wedge peridotite. This mechanism may be triggered by the slab rollback process in a subduction-related environment. Our new investigations, along with available observations from other scholars, support the persistent subduction-related system along the northwestern margin of the Yangtze Block during the early Neoproterozoic.