The removal of tritiated water (HTO) from "ALPStreated water" originating from the disabled Fukushima Daiichi Nuclear Power Plant (FDNPP) is an important environmental issue. In this paper, we report a new method of separating HTO from light water (H 2 O) based on membrane distillation by gas− liquid exchange. HTO-containing water loaded on a hydrophobic membrane modified with a photothermal black dye was exposed to artificial sunlight. The heat generated from the dye upon sunlight exposure vaporized the water, with the HTO-containing water vapor penetrating through the membrane. The permeated HTOcontaining water vapor was mixed with H 2 O added to hydrophilic filters under the membrane. Gas−liquid exchange occurred in these filters and significantly decreased the percentage of HTO in the water collected under all filters. The increases in both the filter number and H 2 O content in the hydrophilic filters increased the efficiency of HTO separation. When four hydrophilic filters containing H 2 O and four hydrophobic filters were set alternately, the ratio of HTO collected under these filters decreased to 12 ± 0.3%. This process was also effective for the removal of 137 Cs from 137 Cs-containing water.