In order to improve the hydrogen storage properties of LiAlH4 and LiNH2, LiAlH4/LiNH2 composite was prepared by ball milling the mixture of LiAlH4 and LiNH2 with Ti or TiF3 as catalyst. The effects of Ti and TiF3 catalyst on the hydrogen storage properties of LiAlH4/LiNH2 composite were studied by thermogravimetry (TG), differential scanning calorimetry (DSC) and X-ray diffraction (XRD) and hydrogen storage properties measurements. The results show that Ti or TiF3 addition significantly improves the desorption kinetics, increases the hydrogen desorption capacity, and decreases the initial hydrogen desorption temperature. For the LiAlH4/LiNH2 composite with addition of 5 mol% TiF3, the hydrogen desorption capacity of the composite increaseses from 1.27 wt% to 1.69 wt% during ball-milling process, the total hydrogen desorption capacity increases from 5.95 wt% to 6.85 wt%, and the initial hydrogen desorption temperature decreases from 150 to 75 oC.