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Deciphering the geochemical diversity of S-type granites is crucial for obtaining more profound insight into their petrogenesis. We therefore undertook an integrated study of whole-rock geochemistry, Sr-Nd isotopes, and zircon U-Pb-Hf isotopes for newly recognized Late Mesoproterozoic S-type granites, including two-mica-, biotite-, garnet-bearing two-mica granites, from the western Yangtze Block, South China. The crystallization ages of these granites are ca. 1040 Ma (weighted mean 206Pb/238U age = 1036.4 ± 4.5 Ma to 1042.2 ± 1.1 Ma). They are peraluminous to strongly peraluminous (A/CNK = molar ratio of Al 2 O 3 /(CaO + Na 2 O + K 2 O) = 1.02–1.67), high-K calc-alkaline rocks, and display high concentrations of normative-corundum (0.54–7.04 wt%) as well as positive correlations of A/CNK and FeOT + MgO values, which are characteristics of S-type granites. These S-type granites are characterized by enriched in Rb, Th, K, and Pb, depleted in Ba, Sr, Ti, and Eu, with negative whole-rock εNd(t) (−0.3 to −6.8) and predominantly negative zircon εHf(t) values (−8.09 to +5.70), indicating the affinity of middle-upper crustal trends and a heterogeneous metasedimentary source. Compared with the geochemical diversity of S-type granites around the world, the variably negative εNd(t) values as well as positive and negative εHf(t) values of our S-type granites may be caused by source heterogeneity and disequilibrium melting processes. More importantly, similar to typical more mafic S-type granites from the Cape Granite Suite (South Africa) and north Queensland (Australia), the high and variable FeOT + MgO contents (2.21–6.64 wt%) are significantly attributed to coupled co-entrainment of peritectic and accessory minerals (e.g., garnet, ilmenite, zircon, and monazite), evidenced by positive relationships between FeOT + MgO and TiO 2 , CaO, Zr, Th, Hf, Y, Yb, light rare earth elements (LREEs). In conjunction with the existence of coeval rift-related A-type igneous rocks, depleted asthenosphere-derived mafic rocks, marine sedimentary sequences, and subsequent extensive Neoproterozoic arc magmatism along the western Yangtze Block, we infer that the ca. 1040 Ma S-type granites studied here were produced in a continental rifting basin that was transformed into a compression setting during the Neoproterozoic. • Late Mesoproterozoic (ca. 1040 Ma) S-type granites in the western Yangtze Block. • They originated from heterogeneous metasedimentary sources. • Source heterogeneity & disequilibrium melting cause heterogeneous Nd-Hf isotopes. • Co-entrainment of peritectic and accessory minerals cause high FeOT + MgO contents. [ABSTRACT FROM AUTHOR]