Three-dimensional network structure of the metal-organic frameworks(MOFs), MIL-53(Cr)as and MIL-53(Al)as, was hydrothermally synthesized by heating a mixture of 1,4-benzenedicarboxylic acid(H2BDC), water, chromium nitrate, and aluminum nitrate for three days at 220 ℃. The samples were then calcinated at 300 ℃ and 330 ℃, respectively, to obtaine MIL-53(Cr)ht and MIL-53(Al)ht. The structure, composition and hydrogen storage properties of the materials were investigated by means of X-ray diffraction (XRD), intelligent weight analyzer (IGA), scanning electron microscopy (SEM), infrared spectrometer (IR) and thermal gravimetric analysis (TG). The results show that the unique breathing effect of the metal-organic frameworks MIL-53, especially the MIL-53(Al)ht which possesses a high surface area, large pore volume and diameter, makes a beter hydrogen absorption performance.