AbstractReturning humans to the Moon presents an unprecedented opportunity to determine the origin of volatiles stored in the permanently shaded regions (PSRs), which trace the history of lunar volcanic activity, solar wind surface chemistry, and volatile delivery to the Earth and Moon through impacts of comets, asteroids, and micrometeoroids. So far, the source of the volatiles sampled by the Lunar Crater Observation and Sensing Satellite (LCROSS) plume has remained undetermined. We show here that the source could not be volcanic outgassing and the composition is best explained by cometary impacts. Ruling out a volcanic source means that volatiles in the top 1-3 meters of the Cabeus PSR regolith may be younger than the latest volcanic outgassing event (~1 billion years ago; Gya).