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Images obtained during MESSENGER's low-altitude campaign in the final year of the mission provide the highest-spatial-resolution views of Mercury's polar deposits. Images for distinct areas of permanent shadow within 35 north polar craters were successfully captured during the campaign. All of these regions of permanent shadow were found to have low-reflectance surfaces with well-defined boundaries. Additionally, brightness variations across the deposits correlate with variations in the biannual maximum surface temperature across the permanently shadowed regions, supporting the conclusion that multiple volatile organic compounds are contained in Mercury's polar deposits, in addition to water ice. A recent large impact event or ongoing bombardment by micrometeoroids could deliver water as well as many volatile organic compounds to Mercury. Either scenario is consistent with the distinctive reflectance properties and well-defined boundaries of Mercury's polar deposits and the presence of volatiles in all available cold traps.