In order to overcome the weak actuation and relaxation problems during the deformation of IPMC actuator, polymeric anion (polystyrenesulfonate)-doped polypyrrole(Ppy(PSS)) was electrodeposited onto IPMC actuator. Electrochemical quartz crystal microbalance study showed that hydrated cations were instilled into Ppy(PSS) film and polymeric-anion dopants introduced during polymerization were not expelled. Ppy(PSS)-coated IPMC actuator formed two electrode/electrolyte interfaces, Pt/nafion and Ppy(PSS)/bulk solution, and additive volume expansion phenomena at interfaces induced the large deformation compensating the relaxation of actuation by back diffusion of water.