The geodynamic model of the paleo-Pacific plate subduction beneath southeastern China during the Late Mesozoic, though generally accepted, remains controversial with respect to the exact plate subduction model. The Moshishan Group volcanic strata are well developed in the Dazhou volcanic basin in the Gan-Hang Belt (GHB). In this study, detailed investigations on geochronology, elemental geochemistry, and isotopic compositions of these volcanic rocks were performed to constrain their formation ages and petrogenesis as well as the tectonomagmatic evolution of the GHB. LA-ICP-MS zircon UPb dating results show that the volcanic eruptions in the Dazhou volcanic basin began approximately 150.9 ± 2.7 Ma to 128.8 ± 1.9 Ma and lasted for ~20 Myr from the Late Jurassic to Early Cretaceous. These volcanic rocks show high Ga/Al ratio, high K₂O + Na₂O and Zr + Nb + Ce + Y contents, and high formation temperature (~812–1022 °C), indicating A-type granite affinity. Such types of A-type volcanic rocks formed in an extensional tectonic environment, likely corresponding to a back-arc extension due to the slab rollback of the paleo-Pacific plate. The ε_Nd(t) values of the volcanic rocks of Moshishan Group vary from −11.60 to −5.41, and the zircon ε_Hf(t) values vary from −18.30 to −3.84, indicating that these volcanic rocks were mainly derived from the partial melting of para-metamorphic rocks. Different proportions of mantle-derived materials were also involved in their sources, such as little or no addition of mantle-derived material in the early Dashuang Formation. However, a significantly increased proportion of mantle-derived material addition was found in the later Gaowu Formation, Xishantou Formation, and Jiuliping Formation. We found that the volcanic rocks in the southwestern GHB were formed during the Early Cretaceous (137–132 Ma), while those in the northeastern GHB formed during the Late Jurassic to Early Cretaceous (150–120 Ma). Jurassic calc-alkaline granites (181–151 Ma) that formed in a continental arc environment related to the paleo-Pacific plate subduction are also distributed along the GHB. This indicates that the shift from an arc environment dominated by the subduction of the paleo-Pacific plate to a back-arc extensional environment characterized by slab rollback began at ~150 Ma in the GHB. We propose an irregular slab rollback model beneath southeastern China to interpret the distribution pattern of the volcanic basins in the GHB. The slab rollback in the GHB did not initiate simultaneously, or with homogeneous velocity, throughout the region. Slab rollback in the southwestern part of the GHB occurred between 137 and 132 Ma, whereas in the northeastern part, rollback occurred between 150 and 120 Ma. In addition, the mantle-crust interaction that produced A-type granitic magmas along the northeastern part of the GHB gradually intensified from the early to late stage between ~150 and ~ 120 Ma.