The invention discloses a novel synthesis method of N, N'-dicyclohexylcarbo-diimide. The novel synthesis method comprises the steps of adding water and cyclohexylamine, starting to stir; dropwise adding carbon disulfide, controlling temperature and pressure, and filtering after cooling to obtain N, N'-dicyclohyxylthiourea; after mixing N, N'-dicyclohyxylthiourea and an adjuvant, adding the mixture into a sodium hypochlorite solution, separating the liquid by heating, adding an organic phase into a hot sodium sulfide solution, separating the liquid while heating, extracting the organic phase, washing the organic phase twice by using a hot sodium hydroxide solution to obtain a crude product, wherein each washing time is 15 minutes; and rectifying to obtain a finished product, namely N, N'-dicyclohexylcarbo-diimide. By using the synthesis method, no organic solvents are used, and the dangers that the organic solvents are flammable and combustible are eliminated; the solvent does not need to be evaporated before N, N'-dicyclohexylcarbo-diimide is rectified, so that the energy waste, the cost and the product loss are reduced, and no solvent residues are left; the novel synthesis method is wide in application range; and the yield and purity of N, N'-dicyclohexylcarbo-diimide are increased, the yield is not lower than 93.5%, and the purity is not lower than 99.3%.