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Piezoelectric materials produce electricity when strained, making them ideal for different types of sensing applications. The most effective piezoelectric materials are ceramic solid solutions in which the piezoelectric effect is optimized at what are termed morphotropic phase boundaries (MPBs). Ceramics are not ideal for a variety of applications owing to some of their mechanical properties. We synthesized piezoelectric materials from a molecular perovskite (TMFM)_x(TMCM)_1–xCdCl₃ solid solution (TMFM, trimethylfluoromethyl ammonium; TMCM, trimethylchloromethyl ammonium, 0 ≤ x ≤ 1), in which the MPB exists between monoclinic and hexagonal phases. We found a composition for which the piezoelectric coefficient d₃₃ is ~1540 picocoulombs per newton, comparable to high-performance piezoelectric ceramics. The material has potential applications for wearable piezoelectric devices.