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The purpose of this work aims at enhancing the electrostrictive strain response and the mechanical energy density under moderate electric field, which is essential for actuator applications. For achieving this, plasticized effects as well as the influence of chlorofluoroethylene and chlorotrifluoroethylene defects on the electromechanical behavior of the copolymer matrix poly(vinylidene fluoride‐trifluoroethylene) (P(VDF‐TrFE)) are investigated. Experimental results showed that the plasticized terpolymer‐based CFE presented better electrical and mechanical performances than the CTFE one. Furthermore, such interesting properties exhibited superior advantages when CFE was combined with (DEHP) plasticizer, resulting in excellent electrostrictive strain response as well as mechanical energy density. Another aspect of this work reports on the influence of the composition, especially the CTFE content, on the electromechanical properties of the neat and plasticized P(VDF‐TrFE‐CTFE). This enables the determination of the desired terpolymer compositions for given applications, which are based on different criteria, such as crystallinity, elastic modulus, dielectric permittivity, and so forth. All the results demonstrated a possibility to realize high performance electroactive polymer actuators while achieving significant improved strain response and energy density under relatively low electric field. Such an investigation allows overcoming the current technological barrier of conventional electroactive polymers that suffer from the high applied electric field usually required to reach sufficient strain. © 2015 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2015, 53, 1368–1379

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