In this study, multilayer graphene (Gr)-reinforced cellulose composites were synthesized by using 1-ethyl-3-methylimidazolium diethylphosphonate ionic liquid. The composites were fabricated via dissolving the cellulose in 1-ethyl-3-methylimidazolium diethylphosphonate and Gr loading at different ratios (0.2, 0.4, and 0.6 wt.%). Both sides of the composites were coated with gold leaf to generate electrodes. The effect of Gr loading on chemical functional groups, crystallographic properties, thermal stability, and morphological and mechanical properties of cellulose film was investigated by Fourier transform infrared spectroscopy, X-ray diffraction, thermogravimetric analysis, scanning electron microscopy, and tensile test, respectively. Electromechanical behavior of the cellulose composite films reinforced with Gr (0.2, 0.4, and 0.6 wt.%) was investigated under DC excitation voltages of 1, 3, 5 and 7 V. Gr loading of 0.2 wt.% increased maximum tip displacement by 400% when the actuator is excited with 3 V.