We fabricated an actuator that was made from polyurethane (PU) with carbon nanotubes (CNTs) as the filler. To improve the dispersion of the CNTs, a mild hydrothermal treatment was carried out. Carboxyl and hydroxyl groups were introduced to the surface of the CNTs, and they were found to be highly dispersed in polar solvents such as dimethylformamide. To evaluate these films, we mainly focused on electrical properties, such as dielectric spectroscopy, space charge measurements, and actuator behavior. We found that the PU/CNTs film bents toward the cathode when an electric field was applied, and it reverted to its original position when the electric field was removed. Upon the inclusion of the CNTs as the filler for the polymer, the electrical properties of the films improved significantly. The highly polarized films had a high relative permittivity, and this produced a higher Maxwell pressure, which assisted the actuation. A high accumulated charge density was observed from space charge measurements in some of the films, and this explains the bending direction and the actuation mechanism.