This paper focuses on actuating mode shapes of cellulose-based electro-active paper (EAPap) in order to investigate its suitability as actuators. Firstly, actuating mechanism of EAPap is addressed based on intrinsic characteristics of cellulose structures under electric fields. EAPap actuator is then fabricated by embedding gold as electrodes into both sides of cellophane sheets. Actuating mode shapes under electric fields are phenomenological measured via laser scanning vibrometer at different exciting frequencies as well as relative humidity. Various actuating performances with large deformations are obtained by applying low electric fields, which can produce a suitable deformation capability with light weight, low power consumption and simple fabrication. Experimental results provide that EAPap can be used as a potential actuating candidate for shape control of smart structures, along with bio-inspired actuator materials.