Methods of nanostructuring and hydrophobization of paint coating surface are studied. It is found that the volume modification of the paint with carbon nanotubes and nanofibers affords nanostructuring of the paint coating surface layer. Additional volume hydrophobization with fluorosilane provides a synergistic effect of the surface superhydrophobicity. Based on the results of the performed investigations, a paint coating possessing superhydrophobic properties has been prepared for the protection of the bottom of marine facilities from fouling.