AbstractQuartz–sillimanite segregations, quartz–albite lithologies (Ab95–98), and Kiruna‐type low‐Ti iron‐oxide deposits are associated with late‐ to post‐tectonic (c. 1055 Ma) leucogranites of Lyon Mountain Gneiss (LMG) in the Adirondack Mountains, New York State. Most recent interpretations of these controversial features, which are global in occurrence, favour hydrothermal origins in agreement with results presented here.Field relations document that quartz–sillimanite veins and nodules cut, and therefore post‐date, emplacement of host LMG leucogranites. Veins occur in oriented fracture networks, and aligned trains of nodules are interpreted as disrupted early veins. Late dykes of leucogranite cut veins and nodules demonstrating formation prior to terminal magmatism. Veins and nodules consist of sillimanite surrounded by quartz that commonly embays wall‐rock feldspar indicating leaching of Na and K from LMG feldspar by acidic hydrothermal fluids. Subsequent, and repeated, ductile flow disrupted earlier veins into nodular fragments but produced little grain shape fabric.Geochemical and petrographic studies of quartz–albite rock indicate that it formed through metasomatic replacement (albitization) of LMG microperthite by sodic hydrothermal fluids that resulted in diagnostic checkerboard albite. Low‐Ti iron‐oxide ores are commonly associated with the quartz–albite sub‐unit, and it is proposed that hydrothermal fluids related to albitization transported Fe as well. The regional extent of sodic alteration suggests large quantities of surface‐derived hydrothermal fluids. Fluid inclusion and oxygen isotope data are consistent with high temperature, regionally extensive fluids consisting primarily of evolved surface‐derived brines enriched in Na and Cl. Quartz–sillimanite veins and nodules, which are significantly more localised phenomena and require acidic fluids, were most likely formed from local magmatic fluids in the crystallizing carapaces of LMG plutons.