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Actuators were developed using activated and non-activated multi-walled carbon nanotube (MWCNT)–ionic liquid (IL) gel electrodes and compared to a single-walled carbon nanotube (SWCNT)-based actuator with respect to the electrochemical and electromechanical properties. The activated MWCNT–COOH/polymer actuator surpassed the SWCNT/polymer actuator in terms of the generated strain.