Oversampled Compact Reconnaissance Imaging Spectrometer for Mars (CRISM) visible and near-infrared hyperspectral data over Mount Sharp in Gale Crater, Mars, were used to generate spatially sharpened maps of the location of red crystalline hematite within the uppermost stratum of an ∼6.5-km-long ridge on the mound’s northern flank. Finely layered strata underlie the ridge to the north and have dips consistent with the nearby Mount Sharp sedimentary sequence. Fe-Mg smectites are exposed in a valley to the south of the ridge. Emplacement of the hematite is hypothesized to result either from exposure of anoxic Fe2+-rich groundwater to an oxidizing environment, leading to precipitation of hematite or its precursors, or from in-place weathering of precursor silicate materials under oxidizing conditions. These hypotheses and implications for habitability will be testable with in situ measurements by the Mars rover Curiosity when it reaches Mount Sharp.