Elucidating the petrological and geochemical characteristics of continental arc crustal fragments can provide unique insights into the magmatic evolutional path and physicochemical conditions (e.g., P−T−H2O) of continental magmatic arcs. This contribution provides a comprehensive set of petrological, mineralogical, geochronological, and geochemical data for the Neoproterozoic Nanba intrusive complex of the western Yangtze Block, South China, which features well-exposed middle−upper crustal sections of the Neoproterozoic continental magmatic arc, to evaluate their magmatic source and fractionation process. The Neoproterozoic Nanba intrusive complex, composed of cumulate gabbros, hornblende gabbros, gabbro-diorites, diorites, granodiorites, K-feldspar granites, and monzogranites, was emplaced at ca. 796−790 Ma. The different lithologies of the Nanba intrusive complex display relatively homogeneous Sr-Nd-Hf isotopes, which indicates a cogenetic evolutional process. The predominantly depleted isotopic characteristics, together with high values of Ba, Rb/Y, and Ba/La, demonstrate that these rocks mainly originated from a subduction fluid−metasomatized mantle source. Petrological and geochemical characteristics, as well as hornblende thermobarometric data, collectively support that the ca. 796−790 Ma Nanba intrusive complex, following the calc-alkaline trend, was dominated by the wet cogenetic fractionation of hornblende accompanied by plagioclase and accessory minerals beneath the middle−upper crustal levels (2.4−4.7 kbar). The cumulate gabbros represent the residue of accumulated hornblende + plagioclase + Fe-Ti oxides from fractionated basaltic melts. The high-SiO2 K-feldspar granites and monzogranites display complementary trace elements, which represent residual silicic cumulates and extracted interstitial liquids in the shallower crystal mush reservoir, respectively. In combination with previous studies, we propose that the middle−upper crustal sections of the Neoproterozoic continental arc of the western Yangtze Block underwent hornblende-dominated fractionation that was followed by significant crystal-liquid separation, which led to the genesis of high-SiO2 melts at the shallower crustal level. The cogenetic evolution played a significant role in molding the petrological and geochemical diversity of Neoproterozoic igneous rocks and the differentiation process of continental arc crust in the western Yangtze Block.