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Addition of an astutely selected third monomer to poly(vinylidene fluoride–trifluoroethylene) (P(VDF‐TrFE))‐based polymers can significantly improve their electromechanical response. This is demonstrated here for the terpolymer containing 1,1‐chlorofluoroethylene as the third monomer, which effectively reduces the all‐trans conformation in the polymer, and thus enhances the molecular conformational changes that accompany the polarization response under an external electric field.