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A layered perovskite-like compound,[C6H5(C2H2)4NH3]2[CuCl4],undergoes a paraferroelastic-ferroelastic phase transition at 337 K,a paraelectric-ferroelectric phase transition at 143 K,and a paramagnetic-ferromagnetic phase transition at 7.5 K,providing a rare new example of single-phase multiferroics.