To comply with green chemistry and achieve sustainable development, an electrically actuated membrane and two non-metallic electrode membranes are assembled into a muscle-like Biomass Hydrogel Paper Actuator (BHPA) similar to ‘sandwich’ structure, which has a great potential in engineering application due to the excellent properties such as light weight, low driving voltage and good flexibility. And the contact resistance between every two membranes of the BHPA is the key factor to improve its output force characteristics and tremor behavior. Thus, in this paper, based on the orthogonal experiment and control variates, under the excitation of electric field, the effect and mechanism of Multi-walled Carbon Nanotube (MWCNT) - Sodium Alginate (SA) based sol-gel coating and its thickness on electrically actuated performances of the BHPA were studied in depth and the results were compared with that of the BHPA samples assembled by the traditional hot laminating technology. Furthermore, with equivalent circuit model, the preliminary quantitative relationship between peak current and contact resistance of the BHPA was derived by a mathematical expression. The results demonstrated that the optimum dimension and testing voltage of the BHPA were 35 mm × 8 mm × 1 layer (0.352 mm) and 4 V, where its output force density and service life both reached the maximum values of 13.34 mN/g and 330 s with the lightest tremor behavior. Moreover, the internal resistance and elastic modulus of the BHPA achieved the minimum values of 2.13 Ω and 3.1 MPa respectively, and its specific capacitance acquired the maximum value of 81.3 mF/g under the sol-gel coating of 1 coating thickness. Generally, it is of great value to modify interface properties of the BHPA for actuation enhancement in demanding working conditions.