A survey–analytical investigation of the adsorption activity of chromium(VI) on the surface of various carbon adsorbents was carried out. The results of physicochemical investigations and their analysis, as well as the data of computer simulations based on quantum-chemical calculations by the standard software packages Gaussian-98 and Firefly 8.0.1, were considered in the study. The features of the possible mechanism of adsorption processes involving chrome(VI) ions and carbon surface were presented.