The invention discloses a preparation method of a Al-InCl3-(Ni-Bi-B) aluminum-based composite hydrogen production material. The material is prepared by mechncial ball-milling mixing of aluminum powder and additives. The additives comprise InCl3 and Ni-Bi-B alloy, wherein the Ni-Bi-B alloy is prepared through dissolving NiCl2.6H2O and BiCl3 in a solvent, adding NaBH4, and carrying out a chemical reduction technology. The preparation method of the aluminum-based composite hydrogen production material comprises the following steps: 1) preparing and drying the Ni-Bi-B alloy; 2) respectively weighing the aluminum powder, InCl3 and Ni-Bi-B in proportion, adding the weighed substances into a ball-milling tank, adding milling balls according to a ball/material ratio, sealing the tank, and filling the tank with argon for protection; and 3) placing the ball-milling tank in a ball mill, setting the ball-milling rotating speed and the ball-milling time, and taking out the prepared aluminum-based composite material. The method has the following advantages: 1, the hydrogen production output under neutral solution and room temperature conditions can reach 1196.8 mL/g, and the hydrogen production rate reaches 100%; and 2, the method has the characteristics of low cost, simple process, highly efficiency in hydrogen preparation, portability in device for implementing the method, hydrogen production and supply at any time, and broad future development and application prospects.