Recently, polyvinyl chloride (PVC) gel materials appeared promising for developing actuators, artificial muscles, and sensors. However, their energized response time and recovery limitations restrict their broader applications. Herein, a novel soft composite gel was prepared by mixing functionalized carboxylated cellulose nanocrystals (CCNs) and plasticized PVC. The surface morphology of the plasticized PVC/CCNs composite gel was characterized by scanning electronic microscopy (SEM). The prepared PVC/CCNs gel composites have increased polarity and electrical actuation with a fast response time. Experimental results demonstrated good response characteristics within the actuator model with a multilayer electrode structure when stimulated with a specified DC voltage (1000 V), with deformation of approximately 36.7%. Moreover, this PVC/CCNs gel has excellent tensile elongation, and the elongation at break of the PVC/CCNs gel is greater than the elongation at break of the pure PVC gel under the same thickness conditions. However, these PVC/CCNs composite gels showed excellent properties and development potential and are directed for broad applications in actuators, soft-robotics, and biomedical applications.