The effect of mechanical activation on the ion-exchange selectivity of natural zeolites from Russia, namely clinoptilolite-bearing tuffs and chabazites, was studied. The structural modifications and thermal properties were investigated, and the specific surface area and porosity of mechanically activated zeolites were determined. At activation doses of up to 1.0 kJ g−1 the main processes are the breakdown of the zeolite particles and pore structure changes. At greater activation doses amorphization takes place. It was shown that during the initial stage of activation in most cases the clinoptilolite selectivity for Sr2+ increased slightly and then decreased; the selectivity for Cu2+ increased 100 times; and the selectivity of chabazite-1 for Sr2+ increased 300 times.