A method of preparing a Cr<3+>-doped CoFe2O4 high-density magnetic-recording material belongs to the technical field of preparation of magnetic-recording materials. In the method, Cr<3+> is doped into metal oxides through a hydrothermal method, so that size of product particles is changed. In a spinel ferrite structure, iron ions are subjected to crystal field to cause quenching of orbital angular momentum, which leads to low magnetic crystal anisotropy and a low coercive force. As a result, by means of the Cr<3+>, of which the orbital angular momentum is not quenched, for doping the CoFe2O4, the CoFe2O4 is improved in magnetic crystal anisotropy. By means of the hydrothermal method, the Cr<3+> is doped with the CoFe2O4, so that two methods of size controlling and element doping are combined, thereby further increasing the coercive force of the magnetic medium. During the process of doping the Cr<3+>, with increase of the doping amount of the Cr<3+>, the product is gradually increased in magnetic crystal anisotropy, and meanwhile, the size of the particles is gradually changed, and when the size is in single-domain critical size range (about 40-100 nm), the product reaches a peak value in the coercive force. The method can further increase the coercive force of the magnetic medium, and is economical and convenient and is easy to popularize.