The invention provides a process for synthesizing biurea by adopting semicarbazide. The process comprises the following steps: a, using semicarbazide and cyanate as raw materials, weighing solid according to the molar ratio of semicarbazide to cyanic acid radicals of 1: (1.01 to 1.05) and adding water; b, keeping the temperature of the mixed solution in a range of 0 to 80 DEG C; c, preparing an acid solution according to the molar ratio of the cyanic acid radical to H+ being 1: (1.01 to 1.05); d, dropwise adding the acid solution into the mixed solution while stirring, and finishing the reaction; and e, filtering, washing and drying. The process has the beneficial effects that firstly, a low temperature is adopted in the reaction, the semicarbazide is stable in property, is difficult to volatilize and is difficult to convert into other substances, the conversion rate is very high, and the yield of 100% can be reached; secondly, a reaction byproduct is sodium salt, has no pollution to the environment, and can be discharged without being post-processed; thirdly, the reaction is performed under a normal pressure and is easy to operate; and fourthly, the acidity is low in the reaction and the equipment is corroded a little.