Cellulose based electroactive paper has been developed as smart material. In this paper, corona poled cellulose films were prepared to improve their piezoelectricity and the influence of grid voltage to the corona poling was investigated. Cellulose was regenerated by dissolving cellulose natural fibers using a solvent, and removing it. During the regeneration process, alignment of cellulose was attempted by applying corona electrical poling. These characteristics were investigated by field emission scanning electron microscopy, transmission electron microscopy, and x-ray diffraction. As increasing the grid voltage of the corona poling, the generation of cellulose nanofibers in the cellulose layered structures was observed, which influenced the increased crystallinity resulting in improved piezoelectric charge constant of cellulose films.