The invention discloses a method for preparing a cyclothiourea compound, which comprises the following steps: suspending a metal hydride in anhydrous THF, stirring, dropwise adding cyclothiourea in the stirring process, stirring at room temperature after adding, then adding diiodobenzene, continuously stirring at room temperature, and monitoring the completion of the reaction by TLC; after the reaction is completed, adding ice water and tetrahydrofuran for a quenching reaction, extracting with ethyl acetate, combining organic layers, washing with a saturated sodium chloride solution, drying with anhydrous sodium sulfate, filtering, spin-drying a solvent, adding a proper amount of silica gel powder for mixing, and performing rapid column chromatography separation to obtain the product, namely the cyclothiourea compound. The method for preparing the cyclothiourea compound by using a reaction system which is free of metal catalysis, cheap in raw material and non-air sensitive is very significant.