The invention discloses a method for directly synthesizing a hydrogen storage material of metal coordination hydride by a reaction ball milling, which is characterized in that metal coordination hydride which is expressed in a chemical general formula as MNH₄ is directly synthesized in a step by the reaction ball milling method and through controlling the hydrogenation pressure and thetime of the ball milling, wherein the chemical general formula, M is one or two of Li and Na, and N is one or two of B and Al, the transition metal such as Ti, Zr and Ni, transition metal halide suchas TiF₃, HfCl₃, TiCl₄, and ScCl₃, rare-earth chloride such as LaCl₃, CeCl₃, PrCl₃, NdCl₃, and SmCl₃ are acted as the catalyst during the synthesis process. The method for directly synthesizing the hydrogen storage material has the advantages of only taking one step of the reaction ball milling to directly synthesize the final product of coordinate metal hydride at a room temperature, having simple operation, low energy consumption, safety, and reliability, enjoying high yield rate of the synthesized hydrogen storage material, and possessing high capacity of reversible hydrogen charging and discharging circulation at a low and intermediate temperature.