Abstract: The high purity metal organic frameworks MIL-101 was prepared by the solvent hot method using 2-methyl imidazole instead of HF acid in this experiment. Ni/MIL101 composite was prepared from the successful load of Ni by the method of excessive impregnation and liquid phase reduction. The product structure, morphology, specific surface area and pore size and thermal stability were characterized via XRD, SEM, BET, TG, FIRT. The hydrogen diffusion coefficient and hydrogen absorption enthalpy of MIL-101 and Ni/MIL-101 composite were measured to investigate the hydrogen storage capacity. The results show that Ni/MIL-101 composite is successfully prepared by this method. The product is a metal skeleton compound with two kinds of pore structure, and the load of Ni can reduce the hydrogen absorption enthalpy of Ni/MIL-101 composite, and the hydrogen diffusion coefficient of Ni/MIL-101 composite reaches 7.6373×10^-7 cm/s, which improves the hydrogen storage capacity of MIL-101.