Nanoscale cobalt-containing nitrogen-doped porous carbon (CoNC) materials were prepared by thermolysis of a zeolitic imidazolate framework (ZIF), ZIF-67, at different temperatures and their application for ionic electro-active polymer (EAP) actuator was evaluated. CoNC-700, which was obtained from ZIF-67 pyrolysis at 700 °C, exhibits specific surface area of 753.86 m2 g−1, pore volume of 0.5768 cm3 g−1, and specific capacitance of 120.7 F∙g−1. CoNC/conducting polymer soft electrode were fabricated by unitizing effective interaction of CoNC with poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS). High-performance ionic actuators were developed for the first time using this CoNC/PEDOT:PSS soft electrode. The developed ionic EAP actuator exhibited large peak-to-peak displacement of 20.4 mm and high bending strain of 0.28% (3 V and 0.1 Hz). Therefore, ZIFs or metal organic frameworks (MOFs) can be applied to provide significant improvements in EAP actuators, which can play key roles as technological advances toward bioinspired actuating devices required for next-generation soft and wearable electronics.