The formation of polymeric self-organizing organosilicon surface nanolayers on copper occuring as a result of modification of the metal surface with organosilane-based formulations has been studied. The anticorrosive effect of such surface layers in corrosive chloride-containing electrolytes as well as in artificial and natural atmospheres has been studied in detail. It has been found that the maximum protective effect is observed at a thickness of 3.8 molecular layers, where the densest cross-linked polymer layers are formed that hinder the adsorption of chloride ions and other corrosive agents on the metal surface, thus significantly reducing the rate of their reactions with the surface copper atoms, and, as a result, inhibiting the corrosion and local anodic dissolution of the metal.