Abstract The flexible actuating behaviors of gel-based artificial muscles (GBAMs) are contingent upon the properties of their hydrogel actuating membranes. While the current preparation system for these membranes is deemed flawless, the electromechanical characteristics are constrained by the inherent properties of the material. The majority of raw materials used in this process are chemically synthesized; however, Chinese herbal polysaccharides offer a convenient, environmentally friendly, and non-toxic alternative, making them a prime candidate for actuating membrane preparation. The biological activities of chamomile polysaccharide (CP) include anti-inflammatory, lipid-lowering, sugar-lowering, and OH- clearance properties. Therefore, the actuating membrane of GBAM was prepared by crosslinking sodium alginate (SA) with CP. The findings indicated that at a crosslinking ratio of 4:5 for CP-SA, the electrically actuated force density and response speed reached 20.12 mN/g and 0.09 mN/g·s, respectively. Additionally, the working life extended to 781 seconds, tremor frequency decreased by 47.67%, and tremor amplitude was 19.55% of the control group. The elastic modulus was measured at 15.44 MPa, specific capacitance reached 183.99 mF/g, and internal resistance decreased by 13.44%. Charge and discharge time was 5.73 seconds, maximum energy reached 2.7 J, and specific energy was 12.66 A·J/g, representing increases of 2.3 seconds, 64.63%, and 6.47 A·J/g compared to the control group. The deflection displacement of 6.62 mm in the CP-SA group at a crosslinking ratio of 4:5 was found to be 3.06 times greater than that of the control group. In conclusion, the actuating membrane of GBAM, synthesized through the cross-linking of CP with SA at a specific ratio, demonstrated superior properties. This innovation offers a novel perspective and direction for the advancement of GBAMs and is anticipated to significantly contribute to future developments in related fields.