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Recently, chitosan is discovered as a most abundant natural polymer, which is not only a lightweight, low‐cost, sustainable resource with potentials in energy transformation, but also biocompatibility and biodegradability. In this article, they investigated a highly biocompatible chitosan‐based electro‐active polymer (C‐Polymer) actuator composed of multiwall carbon nanotube, ionic liquid, and polymer‐supported chitosan. As a result, after the changed MCNTs rate (20%, 40%, 60%, and 80%) in the electrode membrane, actuation properties of C‐polymer actuator behaved a great enhancement. With the increase of the ratio of MCNTs, the specific capacitance and the electrode resistance were obviously improved, which were 2.02 F/g and 1.32 Ω under rate of 80%, and the maximum displacement and the response speed behaved a peak value of 7 mm (80%) and 0.032 mm/s (80%). Interestingly, it also showed an increasing for the maximum blocking force and response speed under the ratio of 80%, which presented the maximum value of 6.80 mN and 0.11 mN/s. In order to analyze causes for this enhancement, a valid generated strain values were calculated to evaluate the strain on the electrode layer. However, it is exhibited that the generated strain was very small, which almost kept in the value of 0.5%, and it was unrelated to Young's modulus. Moreover, they also found that the resistance and the specific capacitance could strongly affect the electromechanical properties of C‐polymer actuator with different rate of MCNTs, and revealed a vital potential Ramsay rule between the electrochemical properties and electromechanical properties of C‐polymer actuator. POLYM. COMPOS., 39:E228–E235, 2018. © 2016 Society of Plastics Engineers [ABSTRACT FROM AUTHOR]