Studies of the lunar atmosphere have shown it to be a stable, low-density surface boundary exosphere for the last 3 billion years. However, substantial volcanic activity on the Moon prior to 3 Ga may have released sufficient volatiles to form a transient, more prominent atmosphere. Here, we calculate the volume of mare basalt emplaced as a function of time, then estimate the corresponding production of volatiles released during the mare basalt-forming eruptions. Results indicate that during peak mare emplacement and volatile release ∼3.5 Ga, the maximum atmospheric pressure at the lunar surface could have reached ∼1 kPa, or ∼1.5 times higher than Mars' current atmospheric surface pressure. This lunar atmosphere may have taken ∼70 million years to fully dissipate. Most of the volatiles released by mare basalts would have been lost to space, but some may have been sequestered in permanently shadowed regions on the lunar surface. If only 0.1% of the mare water vented during these eruptions remains in the polar regions of the Moon, volcanically-derived volatiles could account for all hydrogen deposits – suspected to be water – currently observed in the Moon's permanently shadowed regions. Future missions to such locations may encounter evidence of not only asteroidal, cometary, and solar wind-derived volatiles, but also volatiles vented from the interior of the Moon.