The invention provides a N-hydroxyphthalimide dysprosium coordination compound and a preparation method thereof. The coordination compound has a following chemical formula: [Dy2(HPI)2(NO3)4(DMF)2], wherein HPI is N-hydroxyphthalimide of which one hydrogen ion is removed. The preparation method comprises the following steps: weighing Dy(NO3)3.5H2O and N-hydroxy-1,8-naphthalimide in a hard glass tube, adding an organic solvent, performing uniform shaking, performing vacuum sealing, performing a reaction under heating condition at 60-80 DEG C for 1-3 days, taking out the reaction product, performing slow cooling to room temperature, performing washing, and selecting pure regular single crystals, and performing natural drying to obtain the N-hydroxyphthalimide dysprosium coordination compound.The method provided by the invention prepares the N-hydroxyphthalimide dysprosium coordination compound from selection of a rare earth ion, design of a single-molecular magnet and optimization of a synthetic route, and improves the performance of the rare earth single-molecular magnet; and the coordination compound is a 4f metal coordination compound with a slow relaxation behavior, and has potential application value in the fields of high-density magnetic memorizers and magnetic films.