The Eureka Valley Tuff, erupted from the late Miocene Little Walker volcanic center, east-central California, includes two major ash-flow sheets: the more voluminous, widespread, and more silicic Tollhouse Flat Member and the overlying By-Day Member. Nonhydrated quartz latitic glasses from the Tollhouse Flat and By-Day Members have, respectively, 65.5 and 63.3 wt percent SiO2 and are extremely rich in large-ion lithophile elements. The K2O contents and K/Rb ratios are 5.3 wt percent and 195 for the Tollhouse Flat glass and 5.5 wt percent and 190 for glasses from the By-Day Member. FeO*/MgO (FeO* = total Fe as FeO) ratios are transitional between values characteristic of basaltic and calc-alkalic suites. Initial 87Sr/86Sr ratios of 0.7054 to 0.7055 are consistent with the pattern of northwestward decrease in 87Sr/86Sr observed for Mesozoic plutonic and Cenozoic volcanic rocks in the western Great Basin and Sierra Nevada provinces. The glasses are higher in Rb than are Mesozoic granitic rocks of the Sierra Nevada batholith that have comparable Sr contents and initial 87Sr/86Sr ratios. Pb isotopic compositions fall at the upper end of arrays found for upper Cenozoic calc-alkalic rocks from the Cascade Mountains and nearly on trends found for rocks of the Sierra Nevada batholith. The moderately high FeO*/MgO ratios, very low Co, Cr, and Ni contents, high Ba/Sr and K/Sr ratios, and approximately 25 percent negative Eu anomalies demonstrate that the glasses are the products of appreciable crystal fractionation. This in turn strongly suggests that the Eureka Valley Tuff was derived from a hypersthene-normative or only slightly quartz-normative parent magma. A model is outlined in which a potassic mafic parent magma was produced by a moderate degree of partial melting of diapirically upwelling, undepleted ultramafic mantle material followed by zone refining of upwelling mantle and other material within the asthenosphere and lithosphere. Extensive fractional crystallization and crystal separation subsequently enriched the melt further in large-ion lithophile elements. The evidence for appreciable plagioclase separation demonstrates that much fractionation took place well within the Earth's crust. The Tollhouse Flat and By-Day Members were erupted from discrete — although closely related — bodies of magma. Lower water and halogen contents of the By-Day magma may have prevented the intratelluric crystallization of biotite and thereby allowed the magmatic liquid to become richer in K and Rb than that of the more highly fractionated Tollhouse Flat Member.