Polymers containing neutral and cationic ion moieties within and pendent to their backbones were prepared. The redox properties of the neutral and cationic iron centers were examined using cyclic voltametry. Photolysis of the organometallic polymers led to decoordination of the cationic cyclopentadienyliron moieties from the polymer backbones. Glass transition temperatures of the resulting ferrocene-based polymers were lower than those of the mixed neutral/cationic polymers.