We have created hybrid organic−inorganic nanoarchitectures by electrodepositing ultrathin (<10-nm-thick) polymer coatings onto nanostructured MnO2 birnessite-type electrodes with surface areas in excess of 200 m2 g-1. By choosing a self-limited growth process, based on the electropolymerization of o-phenylenediamine, the resulting polymer conformally coats the oxide nanoscale network without di...