Though there are many stimuli-responsive polymer actuators based on synthetic polymers, electroactive natural biopolymer actuators are very rare. We developed an electrospun fullernol-cellulose biocompatible actuator with much lower power consumption and larger electromechanical displacement in comparison with a pure cellulose acetate actuator. Morphology of the electrospun membranes resembles the nanoporous structure of extracellular matrix in natural muscles. Presence of minute concentrations of fullerenol leads to sharp increase in the degree of crystallinity and substantial increase in tensile strength of membranes. Chemical interactions between cellulose acetate and fullerenols are confirmed by three shifts in carboxylate, carboxy, and carbonyl linkages from the Fourier-transform infrared spectrometry. Much larger tip displacement, nearly 3-fold even at 0.5 wt % fullerenol content, was observed with much lower power I consumption under both alternating and direct current conditions.