Pegmatites are important reservoirs of lithium resources. There is an ongoing debate as to whether Li-mineralized pegmatites were generated from evolved granitic systems via extreme differentiation or by direct melting of metasedimentary rocks. The Chinese Altay is one of the largest pegmatite provinces in the world, and includes many rare-metal pegmatites (e.g., Koktokay, Kelumute, Kaluan and Azubai). However, they display significant differences in formation ages and isotopic compositions compared with the neighbouring or potential parental granites. In this contribution, we present a case study of the Kaluan Li ore deposit in the Chinese Altay, elucidating the origins of pegmatites and related Li mineralization. The Kaluan Li-mineralized pegmatites are characterized by high SiO₂, K₂O, Na₂O, Li, Cs, Ta, and Rb contents; low Fe₂O₃^T, MgO, Ba, and Sr contents; and peraluminous signatures. They have homogeneous HfLi isotopic compositions (ε_Hf (t) = −0.6 to +2.5; δ⁷Li = +1.6 to +5.8‰) that are within the range of HfLi isotopic compositions of the Kulumuti Group schists (ε_Hf (t) = −2.8 to +7.5; δ⁷Li = −8.6 to +10.8‰). In addition, the chemical compositions of the melt derived from the partial melting of the Kulumuti Group by phase equilibrium modeling are compatible with our analyses of the Kaluan Li-mineralized pegmatites. These similarities suggest that the Kaluan Li-mineralized pegmatites were derived from the partial melting of the Kulumuti Group schists at depths during the Triassic, in a post-orogenic and extensional setting. The generation of these pegmatites was mostly controlled by biotite dehydration melting at relatively high temperatures, rather than by the low-temperature melting of muscovite. Trace elements modeling results show that approximately 33–36% partial melting of the average Kulumuti Group schist may produce melts with maximum Li concentrations ranging from 664 to 751 ppm. Subsequently, a high degree of fractionation exceeding 85%, was required for the Li concentration of the residual melt to reach concentrations suitable for crystallization into albite-spodumene pegmatites. Based on our research, an anatectic origin model may have general applicability in explaining the genesis and mineralization of rare-metal pegmatites in the Chinese Altay.