The Sepikou region is located in the eastern Bogda Mountains of the east Tianshan. The Bogda belt is mainly composed of Carboniferous strata, including the Lower Carboniferous Qijiaojing Formation (C1q), Upper Carboniferous Liushugou Formation (C2l), and Qijiagou Formation (C2qj). Here, we report the petrology, geochemistry, and geochronology of bimodal volcanic rocks from the Upper Carboniferous Liushugou Formation, which is widely distributed in the Sepikou region. The basalts, basaltic andesite, and keratophyre have similar petrochemical characteristics and exhibit the high-Na, low-K characteristics belonging to calc-alkalic rocks. These are characterized by the high abundance of K, Rb, Th, Ba, the depletion of HFSE (Nb, Ta, Zr, and Hf), and the slight depletion of Ti. Chondrite-normalized rare-earth elements (REE) patterns for basalts-keratophyre show right-leaning parallel curve clusters, together with a slight enrichment in light rare-earth elements (LREE) contents and low heavy rare-earth elements (HREE)/LREE ratios. The keratophyre exhibits slightly negative Eu anomalies. Compared with the basalts, the rhyolites have high alkali contents, slightly high ∑REE contents, low heavy rare-earth elements/LREE ratios, negative εSr(t) (−9.1 to −12.0), low 87Sr/86Sr initial ratio, highly positive εNd (t) (+5.3 to +6.4), and low Pb isotope ratios. The fractionated REE patterns with prominent negative Eu anomalies suggest they were chiefly derived from the mantle magma underplated basaltic body remelting from the depleted mantle source. The LA-ICP-MS analysis on zircons from quartz keratophyre and rhyolite yield similar ages of 314.9 ± 1.2 and 314.0 ± 1.1 Ma, respectively, suggest that the major bimodal volcanism took place in the Late Carboniferous epoch. The quartz keratophyre zircons, with the 176Hf/177Hf ratios of 0.282897–0.283097, have highly positive εHf (10.99–19.97) and depleted mantle model ages between 180 and 628 Ma. The mafic rocks were chiefly derived from the depleted mantle with the partial incorporation of crustal components. The bimodal volcanic rocks were formed under a continental rift setting. The rift experienced extension in the early period of the Early Carboniferous and its final closure arose after a late period of the Late Carboniferous.