Abstract: Li-mica (zinnwaldite and/or lepidolite)—topaz—albite granites in the Tregonning—Godolphin pluton and similar rocks in the St. Austell pluton appear to be petrogenetically unrelated to the spatially associated biotite granites. Evidence is provided by lack of development of Li-mica granites at roof zones of biotite granites and markedly different trends and composition fields in bivariate plots such as Li vs. Cs, Rb vs. Sr and Nb vs. Zr. Thus, differentiation of biotite granite magma is unlikely to have generated Li-mica granite magma, as also, on its own, is partial melting of biotite granite or biotite-absent residual lower crust. However, partial melting of biotite-rich residual rocks involving biotite breakdown could yield a trace alkali- and F-enriched melt, although this would require marked femic mineral, K-feldspar and anorthite fractionation, and Na-enrichment. It is proposed that volatiles derived from either a mantle source or the crust/mantle interface have aided metasomatism of either residual S-type crust that earlier provided S-type biotite granite magma, or basic (biotite-rich) granitoid, to produce a low-temperature, low-viscosity Li-mica granite melt that rose rapidly in the crust soon after the emplacement of associated biotite granites.