The Sierra La Primavera, near Guadalajara, Mexico, is a Late Pleistocene rhyolitic center consisting of lava flows and domes, ash flow tuff, air fall pumice, and caldera lake sediments. All eruptive units are high-silica rhyolites, but systematic compositional differences correlate with age and eruptive mode. The earliest lavas erupted approximately 145,000 years ago and were followed approximately 95,000 years ago by the eruption of about 20 km3 of magma as ash flows that form the Tala Tuff. The Tala Tuff is zoned from a mildly peralkaline first-erupted portion enriched in Na, Rb, Cs, Cl, F, Zn, Y, Zr, Nb, Sb, HREE, Hf, Ta, Pb, Th, and U to a metaluminous last-erupted part enriched in K, LREE, Sc, and Ti; Al, Ca, Mg, Mn, Fe, and Eu are constant within analytical errors. Collapse of the roof zone of the magma chamber led to the formation of a shallow 11-km-diameter caldera in which lake sediments began to collect. The earliest postcaldera lava, the south-central dome, is nearly identical to the last-erupted portion of the Tala Tuff, whereas the slightly younger north-central dome is chemically transitional from the south-central dome to later, more mafic, ring domes. This sequence of ash flow tuff and domes represents the tapping of progressively deeper levels of a zoned magma chamber 95,000¿5,000 years ago. Sedimentation continued and a period of volcanic quiescence was marked by the deposition of some 30 m of fine-grained ashy sedimients. Approximately 75,000 years ago a new group of ring domes erupted at the southern margin of the lake. These domes are lapped by only 10--20 m of sediments as uplift resulting from renewed insurgence of magma brought an end to the lake. This uplift culminated in the eruption, beginning approximately 60,000 years ago, of aphyric lavas along a southern arc. The youngest of these lavas erupted approximately 30,000 years ago. The lava that erupted 75,000, 60,000, and 30,000 years ago became decreasingly peralkaline and progressively enriched only in Si, Rb, Cs, and possibly U with time. They represent successive eruption of the uppermost magma in the postcaldera magma chamber. Eruptive units of La Primavera are either aphyric or contain up to 15% phenocrysts of sodic sanidine?quartz ≫ferrohedenbergite>fayalite>ilmenite¿titanomagnetite. Major element compositions of sanidine, clinopyroxene, and fayalite phenocrysts vary only slightly between eruptive groups, but the concentrations of many trace elements change by factors of 5--10. This is reflected in phenocryst/glass partition coefficients that differ by factors of up to 20 between successively erupted units. Because the major element compositions of the phenocrysts and the pressure, temperature, and fO2 of the magmas were essentially constant, the large variations in partitioning behavior are thought to result from small changes in bulk composition of the melt. Crystal settling and incremental partial melting are by themselves incapable of producing either the chemical gradients within the Tala Tuff magma chamber or the trends with time in the post-95,000-year lavas. Rather, diffusional processes in the silicate liquid are thought to have been the dominant differentiation mechanisms. The zonation in the Tala Tuff is attributed to transport of trace metals as volatile complexes within a thermal and gravitational gradient in a volatile-rich but water-undersaturated magma. The evolution of the postcaldera lavas with time is thought to involve the diffusive emigration of trace elements from a relatively dry magma as a decreasing proportion of network modifiers and/or a decreasing concentration of complexing ligands progressively reduced octahedral site availability in the silicate melt.