In order to fully utilize Li isotopes as a geochemical tracer, it is necessary to characterize the Li isotopic compositions of different geological reservoirs, and quantify the magnitude of isotopic fractionations for various conditions and compositions. However, our knowledge of Li isotope geochemistry is mostly limited to the hydrosphere and mantle. Little is known about either the Li isotopic composition of the continental crust or the mechanisms by which Li isotopes are fractionated. The primary objective of this thesis is to characterize the Li isotopic composition of the continental crust. Over 50 upper crustal rocks including loess, shale, granite, and upper crustal composites, have been measured and show a limited range of Li isotopic composition (-5 to +5), with an average (0 ± 2 at 1s) that is lighter than the average upper mantle (+4 ± 2). More than 70 high-grade metamorphic rocks, including granulite xenoliths and composite samples from high-grade metamorphosed terranes.