Accurate estimates of global concentrations of Th, K, and FeO have an important bearing on understanding the bulk chemistry and geologic evolution of the Moon. We present empirical ground-truth calibrations (transformations) for Lunar Prospector gamma-ray spectrometer data (K and Th) and a modified algorithm for deriving FeO concentrations from Clementine spectral reflectance data that incorporates an adjustment for TiO2 content. The average composition of soil samples for individual landing sites is used as ground-truth for remotely sensed data. Among the Apollo and Luna sites, Apollo 12 and 14 provide controls for the incompatible-element-rich compositions, Apollo 16 and Luna 20 provide controls for the feldspathic and incompatible-element-poor compositions, and Apollo 11, 15, and 17, and Luna 16 and 24 provide controls for Fe-rich compositions. In addition to these Apollo and Luna sample data we include the composition of the feldspathic lunar meteorites as a proxy for the northern farside highlands to extend the range of the calibration points, thus providing an additional anorthositic end-member composition. These empirical ground-truth calibrations for Lunar Prospector Th and K provide self consistency between the existing derived data and lunar-sample data. Clementine spectral-reflectance data are used to construct a TiO2-sensitive FeO calibration that yields higher FeO concentrations in areas of high-Fe, low-Ti, mare-basalt-rich surfaces than previous FeO algorithms. The data set so derived is consistent with known sample compositions and regolith mixing relationships. Copyright (C) 2004 Elsevier Ltd.