A polypyrrole (PPy)–zigzag metal wire composite film actuator, prepared electrochemically from a methyl benzoate solution of tetrabutylammonium trifluoromethanesulfonate (TBACF3SO3), showed up to 21.4% electrochemical strain, much larger than that (12.8%) of the corresponding PPy–CF3SO3−, driven in aqueous NaPF6 solution.