Graphite is a strategically scarce resource, and the preparation of high-purity graphite is the prerequisite and basis for the application of graphite. In order to determine the optimal purification technology parameters of an ultra-large flake graphite mine pneumatic separation ore with a fixed carbon content of 77.69%, a particle size of mainly 10 to 40 mesh, and main impurities of calcium carbonate, iron oxide and silica , two additional experiments of acid method and alkali method were added on the basis of alkali-acid method, to investigate the purification effect of different technological processes and acid leaching times on graphite raw materials, as well as to analyze the retention extent of different methods and alkali fusion temperature on graphite ultra-large flake structure. The results show that all three methods can increase the fixed carbon content of graphite to above 99%. However, compared with the acid method and the alkali method, the alkali-acid method can obtain high-purity graphite while also better protecting the graphite's ultra-large flake structure. The optimal fusion temperature is 400 °C, the optimal acid leaching time is 30% sulfuric acid thrice and 5% hydrofluoric acid once. After purification, the fixed carbon content of the product exceeds 99.97%.