Investigations on reversible phase transition of coo‐rdination compounds have attracted much interest because they are promised to have wide application on energy storage, temperature controlling, data communication, ferroelastic and ferroelectric materials. Here we report the ferroelastic property, dielectric and heat anomalies of [Zn(en)3]SO4, 1 (en=ethylene diamine).1undergoes two sequential reversible phase transitions. The firestone occurs in the vicinity of 134 K, attributing to the order‐disordered motion of SO42−ions. The second one happens at 202 K, which origins form the symmetry improvement in the trigonal crystal system. Its switchable dielectrical bistability between high and low dielectric states accompanying with large entropy changes (ΔS=10.18 J⋅mol−1⋅K−1) for the phase transitions was confirmed by dielectric and differential scanning calorimetry (DSC) measurements.
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