The invention discloses a Tb, Cr and Mn ternary co-doped high-remanent-polarization BiFeO3 film and a preparation method thereof. The preparation method comprises the following steps: dissolving bismuth nitrate, ferric nitrate, terbium nitrate, chromic nitrate and manganese acetate according to a molar ratio of (0.91-0.97):(0.98-x):(0.08-0.14):0.02:x in a mixed solution of ethylene glycol monomethyl ether and acetic anhydride and uniformly stirring, thus obtaining a BiFeO3 precursor solution, wherein the total metal ion concentration in the BiFeO3 precursor solution is 0.1-0.5mol / L, and x is equal to 0.01 to 0.04; spin coating the BiFeO3 precursor solution on an FTO / glass substrate to prepare a wet film, baking the wet film to obtain a dried film, annealing at the temperature of 550 DEG C for 8-13 minutes, thus obtaining a crystalline-state BiFeO3 film; and after the crystalline-state BiFeO3 film is cooled, repeating the operations until the BiFeO3 film reaches the needed thickness, thus obtaining the Tb, Cr and Mn ternary co-doped high-remanent-polarization BiFeO3 film. According to the method, a sol-gel process is adopted, the equipment requirement is simple, the method is suitable for preparing films on large surfaces and out-of-shape surfaces, the chemical constituents are accurately controlled, and the crystal structure is regulated through co-doping, so that the ferroelectric properties of the film are greatly improved.