We report cellulose-based electro-active paper (EAPap) actuator formed by electrospinning. Cellulose is one of the most abundant natural polymers and has become an attractive smart material. To prepare electrospun nanofibrous cellulose membrane, the LiCl/N,N-dimethylacetamide (DMAc) solvent system was used. The presence of residual LiCl in electrospun membrane was confirmed by elemental analysis using energy dispersive X-ray spectroscopy. To induce orientation, the cellulose membrane was mechanically aligned in simple extension. FE-SEM was used to observe the morphology of the oriented electrospun membranes. The orientation and crystallinity of the cellulose membrane were examined by WAXD. The electro-active characteristic of the electrospun cellulose membrane was measured by the cyclic bending displacement test under different voltages. Aligning of the electrospun membrane was found necessary to render electro-active characteristic.