Albite gneisses containing up to 8.7 percent Na2O and as little as 0.1% K2O comprise a significant part of the Proterozoic Lyon Mountain Gneiss in the Ausable Forks Quadrangle of the northeastern Adirondacks, New York State. Two distinct types of albite gneisses are present. One is a trondhjemitic leucogneiss (LAG) consisting principally of albite (Ab95–Ab98) and quartz with minor magnetite and, locally, minor amounts of amphibole or acmiterich pyroxene. LAG probably originated by metamorphism of a rhyolitie or rhyodacitic ash-flow tuff with A-type geochemical affinities, following post-depositional analcitization in a saline or saline-alkaline environment. The other type is a mafic albite gneiss (MAG) containing albite and pyroxene along with 0–45 percent quartz, minor amphibole, and titanite. MAG locally displays pinstripe banding and contains albite (Ab98) megacrysts up to 5 cm across. Its precursor may have been a sediment composed of diagenetic analcite or albite, dolomite, and quartz. Both types of albite gneiss are interlayered with granitic gneisses (LMG) of variable composition derived from less altered tuffs. A potassium-rich (up to 9.7% K2O) microcline gneiss facies may have had a protolith rich in diagenetic K feldspar. We propose that the albite gneisses and associated granitic gneisses are the granulite-facies metamorphic equivalent of a bimodal, dominantly felsic, volcanic suite with minor intercalated sediments, probably including evaporites. The volcanics were erupted in an anorogenic setting, such as an incipient or failed intracontinental rift. Deposition took place in a closed-basin, playa lake environment, where diagenetic alteration resulted in redistribution of the alkalis and strong oxidation.