Measurements of surface reflectance of permanently shadowed areas near Mercury's north pole reveal regions of anomalously dark and bright deposits at 1064-nanometer wavelength. These reflectance anomalies are concentrated on poleward-facing slopes and are spatially collocated with areas of high radar backscatter postulated to be the result of near-surface water ice. Correlation of observed reflectance with modeled temperatures indicates that the optically bright regions are consistent with surface water ice, whereas dark regions are consistent with a surface layer of complex organic material that likely overlies buried ice and provides thermal insulation. Impacts of comets or volatile-rich asteroids could have provided both dark and bright deposits.