The significance of toxic metals pollution treatment has become incrementally manifested as an important environmental issues in the recent years due to the urgent need to access healthy water and increase of the anthropogenic activities in water contamination. For efficient treatment of water contaminants, the selective and novel materials are always welcomed. In this study, the hydrothermally synthesized titanate nanotubes (TNT) were modified by the mercaptosilane modifier for the removal of Cu(II) and Ni(II) toxic contaminants. The modified TNT adsorbent (TNT/Sil) was characterized in terms of the physicochemical aspects and then, the experiments for capturing metal cations were performed in batch mode. The modified adsorbent presented more affinity for the removal of Cu(II) than Ni(II). The results demonstrated that the experimental data were highly fitted to the Freundlich isotherm model and the maximum uptake capacities for Cu(II) and Ni(II) were found to be 53.77 and 45.29 mg g-1, respectively. In addition, endothermic nature of the adsorption process was predicted by the thermodynamic study as well as the pseudo-second order model that was corresponded to the kinetic data. Considering these achievements and due to the surface hydroxyl and thiol functional groups, TNT/Sil adsorbent could be effective and promising material in the purification of wastewaters, contaminated with toxic metal cations.