The invention provides a preparation method of ultrathin graphite phase carbon nitride. The preparation method comprises steps as follows: melamine is calcined firstly, and blocky g-C3N4 is obtained; blocky g-C3N4 is uniformly dispersed in deionized water and subjected to ultrasonication; a product obtained after ultrasonication is subjected to centrifugal separation, and solids are collected and dried; finally, a dried product is calcined again, and a target product is obtained. According to the preparation method of ultrathin graphite phase carbon nitride, mass preparation and thickness regulation of ultrathin g-C3N4 with the thickness of 0.8-1.2 nm equal to the thickness of 3-4 atom layers are realized, no organic solvent or toxic chemical reagent participates in a reaction process, so that the problems of structure defects and environmental pollution which are caused by introduction of impurities can be effectively solved, and on the basis of the non-toxic characteristic of prepared g-C3N4, the preparation method can be widely applied to photocatalysis, electro-catalysis, biosensing, bioimaging and spintronics. The whole preparation process is simple to operate, high in controllability, good in repeatability, green, environment-friendly and suitable for large-scale production.