The article presents the general pattern of the combined process of oxidative decomposition of organic components of simulated nuclear power plant (NPP) drain water and sorption interaction of the imitators of main dose-forming radionuclides (Cs – radiolabel for 137Cs; stable isotopes of Co, Sr, Mn salts) on natural bentonites from the Cherkasy deposit in presence of sorption-reagent compounds — iron (II) and manganese (II) salts. Hydroxides, oxyhydroxides and oxides of Fe and Mn formed during ozonation are predominantly localized on the surface of bentonite. The chemical composition of the main elements of bentonite after drain water ozonation with the addition of iron and manganese salts remains almost the same as that of natural bentonite. The phase composition of bentonite is presented by the main rock-forming mineral montmorillonite and secondary mineral quartz. The iron-containing phases of the ozonised bentonite are Fe(II)- Fe(III) layered double hydroxides (Green Rust), goethite α-FeOOH and magnetite Fe3O4, and the manganese-containing phases are hausemannite Mn3O4, manganese oxide (II) and manganese oxyhydroxide MnO(OH)2. The iron- and manganese-containing phases deposited on the bentonite surface during ozonation are predominantly weakly crystallized or amorphized structures. At the concentration of salts of iron (50 mg/dm3) and manganese (100 mg/dm3) in the drain water, the specific surface area of bentonites with the formed layer of iron and manganese hydroxides, (oxy)hydroxides and oxides increases compared to natural bentonite (34.2 m2/g) and equals to 55 and 51 m2/g, respectively. The degree of radionuclide removal during ozonationof the simulated solution with the initial concentration of cations (Fe2+ — 5 mg/dm3; Mn2+ —10 mg/dm3; Ca2+ — 5 mg/dm3) in the presence of natural bentonite is 137Cs — 78% ± 2%, Sr2+ —97.55% ± 1%, Co2+ — 96.5% ± 1%, Mn2+ — 99.7% ± 0.5%. To preserve the efficiency of 137Cs and Co2+ radionuclide removal, the initial concentration of cations in the solution can be increased to the following values: Fe2+ — 50 mg/dm3, Mn2+ — 100 mg/dm3, Ca2+ — 50 mg/dm3, and to: Fe2+ —500 mg/dm3, Mn2+ — 1,000 mg/dm3, Ca2+ — 500 mg/dm3 for Sr2+ and Mn2+ removal.