We present new optical (0.4–0.65 μm) spectra of Mercury and lunar pure anorthosite locations, obtained quasi-simultaneously with the Nordic Optical Telescope (NOT) in 2002. A comparative study is performed with the model of Lucey et al. (2000, J. Geophys. Res. 105, 20297–20305, and references therein) between iron-poor, mature, pure anorthosite (>90% plagioclase feldspar) Clementine spectra from the lunar farside and a combined 0.4–1.0 μm mercurian spectrum, obtained with the NOT, calculated for standard photometric geometry. Mercury is located at more extreme locations in the Lucey ratio-reflectance diagrams than any known lunar soil, specifically with respect to the extremely iron-poor mature anorthosites. Though quantitative prediction of FeO and TiO 2 abundances cannot be made without a more generally applicable model, we find qualitatively that the abundances of both these oxides must be near zero for Mercury. We utilize the theory of Hapke (2002, Icarus 157, 523–534, and references therein), with realistic photometric parameters, to model laboratory spectra of matured mineral powders and lunar soils, and remotely sensed spectra of lunar anorthosites and Mercury. An important difference between fabricated and natural powders is the high value for the internal scattering parameter necessary to interpret the spectra for the former, and the requirement of rough and non-isotropically scattering surfaces in the modelling of the latter. The mature lunar anorthosite spectra were well modelled with binary mixtures of calcic feldspars and olivines, grain sizes of 25–30 μm and a concentration of submicroscopic metallic iron (SMFe) of 0.12–0.15% in grain coatings. The mercurian spectrum is not possible to interpret from terrestrial mineral powder spectra without introducing an average particle scattering function for the bulk soil that increases in backscattering efficiency with wavelength. The observed spectrum is somewhat better predicted with binary mixture models of feldspars and pyroxenes, than with single-component regoliths consisting of either albite or diopside. Correct spectral reflectance values were predicted with a concentration of 0.1 wt% SMFe in coatings of 15–30 μm sized grains. Since reasonable cosmogonical formation scenarios for Mercury, or meteoritic infall, predict iron concentrations at least this high, we draw the conclusion that the average grain size of Mercury is about a factor of two smaller than for average returned lunar soil samples. The 0.6–2.5 μm spectrum of McCord and Clark (1979, J. Geophys. Res. 178, 745–747) is used to further limit the possible range of mineralogical composition of Mercury. It is found that an intimately mixed and matured 3:1 labradorite-to-enstatite regolith composition best matches both the optical and near-infrared spectra, yielding an abundance of ∼1.2 wt% FeO and ∼0 wt% TiO 2.