Granitic pegmatites are commonly thought to form by fractional crystallization or by liquid immiscibility of granitic magma; however, these proposals are based mainly on analyses of fluid and melt inclusions. Here, we use the Jiajika pegmatite deposit, the largest spodumene deposit in Asia, as a case study to investigate ore forming processes using isotope dating. Dating of a single granite sample from the Jiajika deposit using multiple methods gave a zircon U–Pb SHRIMP age of 208.4 ± 3.9 Ma, an 40Ar/39Ar age for muscovite of 182.9 ± 1.7 Ma, and an 40Ar/39Ar age for biotite of 169.9 ± 1.6 Ma. Based on these dating results and the 40Ar/39Ar age of muscovite from the Jiajika pegmatite, a temperature–time cooling track for the Jiajika granite was constructed using closure temperatures of the different isotope systems. This track indicates that the granite cooled over ~40 m. y., with segregation of the pegmatite fluid from the granitic magma at a temperature of ~700°C. This result suggests that the Jiajika pegmatite formed not by fractional crystallization, but by segregation of an immiscible liquid from the granitic magma. When compared with fractional crystallization, the relatively early timing of segregation of an immiscible liquid from a granitic magma can prevent the precipitation of ore-forming elements during crystallization, and suggests that liquid immiscibility could be an important ore-forming process for rare metal pegmatities. We also conclude that isotope dating is a method that can potentially be used to determine the dominant ore-forming processes that occurred during the formation of granite-related ore deposits, and suggest that this method can be employed to determine the formation history of the W–Sn ore deposits found elsewhere within the Nanling Metallogenic Belt.