Leucogranites in the Lalong Dome are composed of two-mica granite, muscovite granite, albite granite, and pegmatite from core to rim. Albite granite-type Be–Nb–Ta rare metal ore bodies are hosted by albite granite and pegmatite. Based on field and petrographic observations and whole-rock geochemical data, highly differentiated leucogranites have been identified in the Lalong Dome. Two-mica granites, albite granites, and pegmatites yielded monazite ages of 23.6 Ma, 21.9 Ma, and 20.6 Ma, respectively. The timing of rare metal mineralization is 20.9 Ma using U–Pb columbite dating. Leucogranites have the following characteristics: high SiO₂ content (>73 wt.%); peraluminosity with high Al₂O₃ content (13.6–15.2 wt.%) and A/CNK (mostly > 1.1); low TiO₂, CaO, and MgO content; enrichment of Rb, Th, and U; depletion of Ba, Nb, Zr, Sr, and Ti; strong negative Eu anomalies; low εNd(t) values ranging from −12.7 to −9.77. These features show that the leucogranites are crust-derived high-potassium calc-alkaline and peraluminous S-type granites derived from muscovite dehydration melting under the water-absent condition, which possibly resulted from structural decompression responding to the activity of the South Tibetan detachment system (STDS). Geochemical data imply a continuous magma fractional crystallization process from two-mica granites through muscovite granites to albite granites and pegmatites. The differentiation index (Di) gradually strengthens from two-mica granite, muscovite granite, and albite granite to pegmatite, in which albite granite and pegmatite are highest (Di = 94). The Nb/Ta and Zr/Hf ratios of albite granite and pegmatite were less than 5 and 18, respectively, which suggests that albite granite and pegmatite belong to rare metal granites and have excellent potential for rare metal mineralization.