A preparation method of a multi-ferric heterojunction thin film is characterized by comprising the steps of 1) combining a ferromagnetic thin film on a stable-structure ferroelectric thin film substrate by methods such as pulse laser deposition, magnetron sputtering or molecular beam epitaxy during preparation of the thin film to obtain a ferromagnetic/ferroelectric heterojunction thin film, wherein the ferroelectric thin film substrate is one or PMN-PT, BFO, PZT, BTO, PTO and PZN-PT, and the ferromagnetic thin film is one of Fe, Co, Ni, CoFe, CoFeB, FeNi, FeSi, FeSiAl and FeAl; and 2) placingthe ferromagnetic/ferroelectric heterojunction thin film prepared in the step 1) in a heat treatment furnace by interface control, introducing a nitrogen-containing gas at a constant rate, performingnitrogen impregnation processing for 0.5-48 hours under a temperature of 150-600 DEG C, reducing a temperature, cooling with the furnace to a room temperature, and taking out a sample, wherein the stable-structure ferroelectric thin film is not affected during the heat treatment process, nitrogen atoms can be impregnated into the ferromagnetic thin film to generate a gap solid solution or a new phase, cause lattice expansion and generate stress at an interface, and the nitrogen-containing gas is one of nitrogen, ammonia, nitrogen and hydrogen and ammonia and hydrogen.