The Kalba–Narym metallogenic belt is located in East Kazakhstan, which displays rare metal mineralization. The Kvartsevoye rare metal Li–Ta–Nb deposit is located in the north-western ore district. This study presents the results of geological, mineralogical, geochemical, and geochronological analyses of rare metal granite pegmatites. Rare metal mineralization belongs to a field of variably differentiated pegmatites, including barren, quartz–albite–muscovite, muscovite, and muscovite–quartz–albite microcline mineral associations. This study established that the rare metal mineralization is localized in the quartz–albite–muscovite zone. The main concentrator minerals of rare metals are spodumene for Li and tantalite–columbite for Ta and Nb. Ar/Ar dating of the muscovite allowed us to establish the age of mineralization during the period of 288–285 Ma. The present study enabled the linkage of rare metal mineralization with the differentiation processes of the granites of the Kalba complex.