Thin CNF/PPy composite single-layer films were produced by the electrophoretic deposition and polymerization process which was developed for this study. It was demonstrated that the films could generate a bending motion subjected to an actuating electric voltage even though they consisted of only single-layer. Carbon nanofiber and polypyrrole composite films were obtained from only one side of a working electrode. Several different CNF/PPy films were synthesized, as varying the CNF weight ratios from 3%, 5%, and 7% to 10%. Conductivity of pure PPy and CNF/PPy composite films were measured. Conductivity of the films is improved linearly from 77.9S/cm (pure PPy film) to 124.3 S/cm (10% CNF/PPy) as the CNF weight ratio increases. Adding CNF was effective for improving the conductivity of PPy. As results of electromechanical actuation tests with the films, it was noticed that the strain of the films was reduced a little as the CNF weight ratio increased. Bending motions were observed for both ppy and CNFIPPy films subjected to a voltage. The tip bending deflections was in the range of 0.5 mm to 2 mm. CNF/PPy films showed a great potential to be a good candidate for small light actuators.