Abstract: Materials and methods of modifying an electrode surface are described herein. Self-assembled monolayers (SAM) of polyaromatic molecules covalently attached and form a graphitic-like surface on the electrode surface. After covalent attachment of the polyaromatic monolayer to the surface, polyaromatic-functionalized molecular species is physisorbed onto the surface using the ?-interactions. This concept can be applied to generate high performance electrode materials modified with molecular species. The electrode materials can be applied in photoelectrochemical cells, electrochemical cells, sensors, and electrochromic materials. This approach overcomes the major synthetic challenges to modifying surfaces with molecular species, in addition to protecting the surfaces from corrosion.