Although grain boundaries can serve as effective sinks for radiation-induced defects such as interstitials and vacancies, the atomistic mechanisms leading to this enhanced tolerance are still not well understood. With the use of three atomistic simulation methods, we investigated defect-grain boundary interaction mechanisms in copper from picosecond to microsecond time scales. We found that grain boundaries have a surprising "loading-unloading" effect. Upon irradiation, interstitials are loaded into the boundary, which then acts as a source, emitting interstitials to annihilate vacancies in the bulk. This unexpected recombination mechanism has a much lower energy barrier than conventional vacancy diffusion and is efficient for annihilating immobile vacancies in the nearby bulk, resulting in self-healing of the radiation-induced damage.