The invention relates to a multiferroic compound and a preparation method thereof. The multiferroic compound is characterized by adopting the molecular formula of [C6H5(C2H2)4NH3]2[CuCl4], adopting a layered perovskite-like structure, and belonging to a tetragonal system at 350 K, and monoclinic systems at 293 K and 120 K, wherein the space group of the tetragonal system at 350 K is P4/mbm, and the cell parameters a, b, c and V of the tetragonal system at 350 K are 7.4531(4) angstrom, 7.4531(4) angstrom, 23.317(2) angstrom, and 1295.2(2) angstrom<3> respectively; the space group of the monoclinic system at 293 K is P2(1)/a, and the cell parameters a, b, c, beta and V of the monoclinic system at 293 K are 7.2620(5) angstrom, 7.4725(6) angstrom,23.282(2) angstrom, 91.999(2) degrees, and 1262.6(2) angstrom<3> respectively; the space group of the monoclinic system at 120 K is P2(1), and the cell parameters a, b, c, beta and V of the monoclinic system at 120 K are 27.663(1) angstrom, 7.4916(5) angstrom, 29.423(2) angstrom, 101.819(2) degrees, and 5968.3(6) angstrom<3> respectively. The multiferroic compound provided by the invention has three basic ferric properties of ferroelasticity, ferroelectricity and ferromagnetism at the same time, and has the advantages that ferroelastic phase transition occurs at a temperature higher than the room temperature; magnetic bistable state occurs during ferroelectric phase transition or ferroelastic phase transition.