In the present paper the mesoporous TiO 2 with chemosorbed carbonate groups was investigated as an adsorbent for the removal of Zn 2+ and Ba 2+ cations from aqueous solutions.The dependence of the adsorption values of Zn 2+ and Ba 2+ on the agitation time, solution's acidity, and modification of surface of TiO 2 was determined. The process of Zn 2+ and Ba 2+ adsorption fit well by Lagergren's pseudo-second-order kinetic model. The equilibrium adsorption was investigated in the concentration of heavy metal's ranges 27.46 mg/L -7809 mg/L. The experimental data was approximated by Langmuir and Dubinin-Radushcevich adsorption theories. The energy of adsorption Zn 2+ and Ba 2+ onto modified TiO 2 and unmodified TiO 2 was calculated using Dubinin-Radushkevich equations, and was found to be 15.82 -9.399 kJ/mol, which corresponds to the mechanism of physical adsorption. The application of Langmuir theory to experimental adsorption data gives high R 2 , close to unit. Separation factor R L indicates, that adsorption Zn 2+ and Ba 2+ onto modified TiO 2 is very favorable.The mechanism of adsorption of bivalent cations by the modified sample is approximately the same. The difference in the adsorption of Zn 2+ compared with Ba 2+ is that cations of Zn 2+ (with small size) can diffuse into the micro pores of modified TiO 2 . The adsorption of Zn 2+ is not so strongly influenced by the presence of Ba 2+ , as in the adsorption of Ba 2+ the presence of Zn 2+ in the solution. This fact can be used for the separation of the Zn 2+ -Ba 2+ pair.Modified mesoporous ТіО 2 is very efficient adsorbent toward Zn 2+ and Ba 2+ cations from their individual solutions as well as from their mixture, and able to compete with the best world analogues.