Rod-like aggregates formed from polymerized surfactant systems form organized two-dimensional layers at the solid-liquid interface. These layers are self-organized during the adsorption of the complexes at the solid surface. In common with layers formed from simple surfactants, the adsorbed layer structures show a high degree of ordering at the nanometer to micron length scales. Unlike their simple surfactant analogues, the layers formed using the polymerized surfactant systems are irreversibly adsorbed and are not sensitive to subtle interactions between the substrate and surfactant molecules. This allows for a wide range of processing options for these nanoorganized films.