To enhance the performance of ionic actuators, the electrochemical and electromechanical properties of green ionic actuators with the electrolyte layer after doping with MWCNT was investigated in this paper. The surface morphology, elemental composition, corresponding content and functional group of the mixed electrolyte layer were observed and characterized by SEM–EDS, FT-IR and XRD. The CV test showed that when the doping amount was 0.8 wt%, the specific capacitance increases 187.6% and 205.3% compared with undoped electrolyte layer at the sweep speed of 20 mV s−1,500 mV s−1, respectively. The GCD test showed that the energy density increased to 144.3% at the current density of 1 A g−1. and the cycle life is correspondingly increased. At 5 V DC, the deflection displacement of actuators was 10.12 mm when the doping amount was 0.8 wt%, which was 238.1% higher than when the doping amount was 1.5 wt%. And the output force of actuators was 3.10 mN, which was 147.2% higher than when the doping amount was 0 wt%. At 5 V/0.05 Hz voltage, the peak displacement of the actuator was 2.871 mm, which was 238.1% higher than when the doping amount was 1.5 wt%.