According to several orbital reflectance spectroscopy studies, numerous widely scattered lunar surface locales feature remarkably high (>98%) abundance of plagioclase. These “pure” anorthosite claims are based on an absorption band at ∼1.25 μm, associated with minor Fe2+ within plagioclase. But utilization of the 1.25 μm band as a direct gauge of plagioclase abundance requires an underlying assumption that plagioclase FeO is uniform across all measured materials. Available data for FeO in lunar plagioclase are in many cases suspect because electron-probe FeO measurements may be inflated by secondary fluorescence from nearby mafic phases. We studied plagioclase FeO in a set of 13 anorthositic lunar rocks, taking care to avoid proximity to mafic phases; or in cases where complete avoidance was not possible without sacrificing representativeness (i.e., fine-grained impact melt rocks with zoned silicates), correcting close-to-mafic analyses for secondary fluorescence (Sugawara, T. [2001], Japanese Mag. Mineral. Petrol. Sci. 30, 159–163). Results for rock-average plagioclase FeO range from 0.030 wt% in plutonic troctolitic anorthosite 76335, to 0.23 wt% in impact-melt rock 14310. In general, as shown by exsolution of mafic silicates from plagioclase within several samples, final plagioclase FeO in lunar plutonic anorthosites is determined by reequilibration during slow postigneous cooling and/or metamorphism. In contrast, four fast-cooled anorthositic impact melt rocks have consistently higher plagioclase FeO, averaging 1.9 times higher in comparison to average plutonic anorthositic rock. Thus, impact melted lunar anorthosite will have far more prominent 1.25 μm absorption than plutonic anorthosite of the same plagioclase abundance. In view of the inconstancy of plagioclase FeO, orbital spectral reflectance using the 1.25 μm absorption band, or the ratio between that band and one or more mafic silicate bands, cannot be precise enough to justify claims of ability to resolve “purest” (98 vol% +) anorthosite from compositions that are high-plagioclase but not that extreme.