The origin and petrogenesis of pegmatite-type lithium deposits within the Songpan-Garze Fold Belt (SGFB) of western China remain subjects of debate. To provide further insight on this subject, this study investigated the whole-rock trace elements and whole-rock Li isotopic compositions of the two-mica monzogranite (TMG) from the Ke’eryin composite pluton, the Jiada albite pegmatite (AP) and albite-spodumene pegmatite (ASP) and their metasedimentary wall rocks within the Ke’eryin ore field in the eastern SGFB. Modeling of muscovite-dehydration melting based on the whole-rock trace elements (e.g., Li, Rb, and Sr) and Rayleigh dehydration modeling related to the whole-rock Li isotopes suggest that the Jiada pegmatites are unlikely to have originated from the low-degree partial melting of metasandstone (MS) of the Zhuwo Formation. Variations in the whole-rock trace elements and Li isotope between the TMG and the Jiada pegmatites are consistent with the evolution trend of magmatic fractionation. However, the whole-rock Li isotopic compositions of the AP and ASP display inverse variation characteristics with the muscovite Li isotopic compositions, with the AP exhibiting lower Li concentrations and higher whole-rock δ7Li values than ASP. Furthermore, the variation patterns of whole-rock trace elements do not align perfectly with the Rayleigh-type fractional crystallization processes, implying other geological processes would be also involved in the formation of the Jiada pegmatites. Collectively considering the Li isotope behavior during various geological processes, the observed variations in whole-rock Li isotopic compositions between AP and ASP can be explained by aqueous fluid enrichment during the pegmatitic melt evolution. This suggests that fractional crystallization and fluid exsolution jointly contributed to pegmatite formation and Li mineralization in the Jiada deposit. Moreover, the whole-rock δ7Li values of the wall rock of ASP (MS2) are lower than those of MS and the wall rock of ASP (MS1), primarily due to metasomatism by 6Li-enriched fluids expelled from ASP and the kinetic diffusion of Li isotopes. The high concentrations of highly mobile elements, especially Li and Cs, combined with the low whole-rock δ7Li value of the metasandstone, could serve as effective tracers for locating concealed orebodies and evaluating the metallogenic potential of Li mineralization.