Sand-sized impactite melt grains hand-picked from a glaciofluvial sample proximal to the Hiawatha impact crater in Northwest Greenland contain new information about the crystallization and cooling history of this impact structure, which is concealed by the Greenland Ice Sheet. Of course, the original locations of the individual sand grains are unknown, but this is offset by the substantial number and wide variety of impactite grains available for study. A detailed investigation of 16 melt grains shows that post-cratering crystallization took place under very variable conditions of strong undercooling with temperatures that dropped rapidly from high above their solidus to far below. A distinct event of near-isochemical hydration at above or ∼250 °C is recorded by intense perlitic fracturing and the growth of closely packed mordenite spherulites only 1−3 μm across in felsic melt grains, which was followed by lower temperature hydrothermal alteration along the pre-existing perlitic fractures. The formation of abundant mordenite microspherulites appears to be very rare or not previously recorded in impactite melts and suggests the rapid infilling of the Hiawatha crater by a hydrous source. The infilling did not occur immediately after the impact as in submarine impacts, but soon thereafter, and before the establishment of a low-temperature hydrothermal alteration system common to the waning stage of cooling in many impact structures. These observations and previous documentation of terrestrial organic matter in the impactites are consistent with an impact into a water-rich terrestrial environment, such as through the Greenland Ice Sheet or into a forested, lacustrine−fluvial region.