Disclosed is a method for making a pure aluminum nitride substrate. At first, aluminum nitride is mixed with a water-resistant material and an adhesive material. The mixture is made into grains in a granulation process. The grains are molded into a nugget in a steel mode by hydraulic pressure. The nugget is subjected to a cold isostatic pressing process. At a low temperature, the water-resistant material and the adhesive material are removed from the nugget. Then, the nugget, boron nitride and nitrogen are introduced into and sintered in an oven, thus providing a pure aluminum nitride substrate. The purity and quality of the aluminum nitride substrate are high. The aluminum nitride substrate can be used in a light-emitting diode. The method is simple, the yield is high, and the heat radiation of the aluminum nitride substrate is excellent.