Herein, an advanced concept to enhance the actuation ability of electroactive polymers (EAPs) based on modified terpolymer P(VDF‐TrFE‐CFE) is proposed. Such a polymer matrix attracts a great deal of attention because of its outstanding electromechanical coupling property, particularly when doped with plasticizers, e.g., diisononyl phthalate (DINP). Herein, it is demonstrated that by optimizing the structure's multilayer design, the electromechanical coupling of the modified terpolymer is enhanced with its high dielectric permittivity, low Young's modulus, and exceptional dielectric strength. This leads to a large strain response as well as a high mechanical energy density at relatively low electric fields according to the electrostriction phenomena. The concept of stacked multilayers is demonstrated as a simple and effective technique to boost the actuation abilities. Experimental results in accordance with numerical models show actuator performance with a large electromechanical response. This technology shows feasibility for active optical surface shape control. The potential of multiple‐stack actuators is tested in a small prototype. This demonstrated mirror optical shape control and correction with a few degrees of freedoms. The proposed Live Mirror technology is useful for ground‐ and space‐based astronomy and communications telescopes.