At Long Valley (LV) model Sr isotope phenocryst ages and absolute U–Pb zircon ages from precaldera Glass Mountain (GM) and caldera-related Bishop Tuff (BT) rhyolites show that these crystals track >1 Myr of evolution of a voluminous rhyolite magmatic system. In detail, strong disparities between the different age populations complicate ideas for a unified model for rhyolite generation, differentiation, and storage. To better elucidate the age discrepancies a new in situ Pb isotope technique has been developed to measure the compositions of 113 individual LV feldspars (mainly sanidine) and their host glasses by UV laser ablation MC-ICPMS. Given sufficient signal the accuracy and precision of this technique approaches that of double-spike thermal ionization mass spectrometry. The utility of our technique for many geologic materials is, however, limited to determining Pb isotope ratios that include 206Pb, 207Pb, and 208Pb, but exclude 204Pb. New zircon 238U– 206Pb crystallization ages were also obtained for two older Glass Mountain domes. A >1.5‰ difference between the Pb isotope compositions of feldspars from older (1.7–2.2 Ma) precaldera Glass Mountain (GM) rhyolites and younger LV rhyolites, including the BT, is found. The Pb isotope data for feldspars and their host glasses lie along a regional trend line between young basalts and evolved crust compositions, spanning ∼15% of that isotopic difference, and show a secular change towards increasing mantle contribution. Most feldspars have Pb isotope compositions that are similar to their host glasses and, as such, there persists an apparent >100 k.y. difference between Sr model feldspar ages and zircon ages for some GM rhyolites. Collectively, the feldspars define a Sr–Pb isotope mixing curve. Evidence for mixing complicates the interpretation that the Sr isotope data solely reflect radiogenic ingrowth. Where isotopically heterogeneous feldspar populations occur, there is greater uncertainty about the veracity of the Sr model ages. Specifically, we find no Pb isotope evidence that BT feldspars grew from older GM-like magmas. The distinct Pb isotope signatures for individual rhyolites and their feldspars support evidence based on zircon dating that LV volcanism did not erupt from a single long-lived magma chamber but rather tapped a number of different magmas. Moreover, contrary to the conventional model of gradual build-up prior to cataclysmic eruption, secular changes in the U–Pb age constraints on magma residence times and the magmas’ distinct Pb isotopic compositions suggest that, at Long Valley, eruptive volumes increase with shorter magma residence time and correlate with greater mantle input. Evidently, the plumbing and therefore activity at Long Valley was influenced by the evolving interaction between source and crustal magma system.