We conducted field investigations, whole-rock geochemical, Sr-Nd and zircon U-Pb-Lu-Hf isotopic analyses on a suite of intrusive complex in the southern Nalati Range, SW Chinese Tianshan in order to better understand the Paleozoic tectonic and magmatic evolution of the belt. The intrusive complex comprises weakly foliated diorite, low-grade altered diabase, and deformed monzogranite; these plutonic rocks were in turn crosscut by undeformed coarse-grained diorite, granodiorite as well as granite stock. Foliated Late Silurian diorites (421 ± 4 Ma) show arc-type geochemical features, slightly negative whole-rock εNd(t) value (− 1.7; T_DM-Nd = 1.52 Ga) and variably positive zircon εHf(t) values (2.34 to 7.27; T_DM-Hf: 0.95– 1.26 Ga). Deformed Early Devonian porphyritic monzogranites (411 ± 4 Ma) show geochemical features similar to A-type granite, and their zircon εHf(t) values range from − 6.63 to 1.02, with T_DM-Hf ages of 1.82 to 1.33 Ga. Metamorphosed Early Devonian diabases (ca. 410 Ma) have OIB-like REE patterns, εNd(t) values of − 2.0 ~ − 0.8 and T_DM-Nd ages of 1.37– 1.25 Ga. The undeformed Early Carboniferous diorite and granodiorite (353– 344 Ma) exhibit arc-type geochemical features, positive εHf(t) values of 6.11– 7.91 with T_DM-Hf ages of 0.97– 0.86 Ga, and positive εNd(t) value of 1.9 with T_DM-Nd age of 1.04 Ga. The Early Permian granite stock (292 ± 5 Ma) has highly differentiated REE pattern, slightly negative εNd(t) value (− 4.4) and variable zircon εHf(t) values of − 9.73– 6.36. Combining with available data, Early Paleozoic (500– 410 Ma) arc-related magmatic rocks occurring on both sides of the suture zone along the southern Nalati Range, likely resulted from a bi-directional subduction of the Paleo-Tianshan Ocean beneath the Yili Block to the north and the Central Tianshan to the south. Occurrences of A-type granites and OIB-like diabases (ca. 410 Ma) along the Nalati Range likely indicate a hot extensional regime probably induced by the break off of the northward subducting slab of the Paleo-Tianshan Ocean. The closure of the Paleo-Tianshan Ocean and subsequent amalgamation during Early Carboniferous resulted in the regional deformation and metamorphism of the Early Paleozoic arc-related magmatic rocks. From Early to Late Carboniferous, a magmatic arc that corresponded to the well-developed Late Paleozoic Balkhash-Yili active continental margin, superimposed upon the southern Yili Block, most likely resulted from the southward subduction of the Junggar-North Tianshan Ocean. After the closure of the North Tianshan Ocean in Late Carboniferous, the study area was dominated by post-orogenic magmatism.