The Kalatag mineralization belt is an important metallogenic belt of polymetallic mineral deposits in the northern part of eastern Tianshan, and its age and tectonic setting are still controversial. We identified a set of Devonian volcanic rocks hosted in the Early Palaeozoic package of dominantly marine sediments with a small amount of terrestrial rocks. This study presents petrological, U–Pb geochronology, and geochemical data for the volcanic rocks. The ages of the rhyolite (407.2 ± 1.9 Ma) and basaltic andesite (380.4 ± 2.8 Ma) suggests that the Kalatag belt is a Devonian volcanic succession. These rocks consist mainly of marine calc–alkaline lava, tuff, pyroclastic rocks, and minor terrestrial basaltic andesite. The lavas are characterized by the enrichment of light rare earth elements and strongly depleted in Nb and Ta, typical of island arc magmatic rocks. The volcanic rocks probably originated from the partial melting of the mafic lower crust which was modified by subducted slab-related fluids. During their ascent through the crust, these volcanic rocks underwent variable extents of fractional crystallization (rhyolites) and crustal contamination (basaltic andesites). Combined with the results of previous studies, we suggest that the Devonian rocks formed in an island arc related to the northward subduction of the Northern Tianshan Ocean with a crustal thickness of ~35–40 km.