The modification of natural zeolites was carried out under hydrothermal conditions to improve the effectiveness of the uptake of ammonium ions. Natural zeolites originating in Japan, such as mordenite and clinoptilolite with quartz, feldspar and a trace of layered silicate, were treated with 0.1, 0.3, 1.0 and 3.0 M NaOH solutions at temperatures from 25 to 150• C under autogenous pressure for 7 days. After the hydrothermal treatment, the transformation of the zeolites to phillipsite, hydroxyl-sodalite and analcime was observed, depending on the temperature and NaOH concentration. The amounts of ammonium ions taken up into the hydrothermally-treated zeolites were compared with those of the starting materials. The treated products, containing mainly phillipsite, took up twice the amount of ammonium ions as the starting materials. The maximum uptake of ammonium ions was 1.92 mmol g −1 . The number of ammonium ions taken up into phillipsite was equal to the number of Na + ions released from phillipsite. These results indicate that the uptake of ammonium ions proceeds by an ion-exchange mechanism with Na + ions.