This study investigates the geological, mineralogical, and geochemical features of the Alday ore occurrence (Central Kalba, East Kazakhstan) and aims to identify indicators of rare-metal mineralization, with lithium considered to be one of its principal components. In this study, the structural–stratigraphic position of the occurrence is refined; three series of albite–spodumene pegmatites are identified; the compositions of the ore-bearing schists and the granitoids of the Kunush and Kalba complexes are compared; and the role of metasomatic alteration in the concentration of Li, Ta, Nb, Be, and Sn is established. The plagiogranites and dikes of the Kunush complex are characterized by Li anomalies (up to 306 g/t), Ta (up to 64 g/t), and a fractionated REE spectrum (La/Yb up to 108). In addition, the following predictive criteria are formulated: the presence of tectonically disrupted dikes in the Kunush complex with Na₂O/K₂O > 4, the presence of albite and muscovite alteration zones, and the presence of ladder-type spodumene-bearing pegmatites controlled by northwest-trending faults. The ⁴⁰Ar/³⁹Ar muscovite age of the Alday pegmatites (~292 Ma) aligns with the age range of the Kalba granite complex. Based on the main principles of rare-metal pegmatite generation, it is determined that the Tochka pegmatites were formed during the fluid–magmatic fractionation of magma in large granitic reservoirs of the Kalba complex. The Karagoin–Saryozek zone—located between several large granite massifs of the Kalba complex, where host rocks function as a roof—may be promising for investigating rare-metal pegmatite mineralization.