We report on the recent progress and development of research into cellulose-based electro-active paper for bending actuators, bioelectronics devices, and electromechanical transducers. The cellulose electro-active paper is characterized in terms of its biodegradability, chirality, ample chemically modifying capacity, light weight, actuation capability, and ability to form hybrid nanocomposites. The mechanical, electrical, and chemical characterizations of the cellulose-based electro-active paper and its hybrid composites such as blends or coatings with synthetic polymers, biopolymers, carbon nanotubes, chitosan, and metal oxides, are explained. In addition, the integration of cellulose electro-active paper is highlighted to form various functional devices including but not limited to bending actuators, flexible speaker, strain sensors, energy harvesting transducers, biosensors, chemical sensors and transistors for electronic applications. The frontiers in cellulose paper devices are reviewed together with the strategies and perspectives of cellulose electro-active paper and cellulose nanocomposite research and applications.