HPSB (Hydrolysis Product of Sodium Borohydride) hydrogen storage material is a kind of porous lamellar structural material developed by our research group. Due to the special structure of this material, it can absorb hydrogen at room temperature, hydrogen absorption pressure is 2–4 MPa, and hydrogen absorption time is 2–5 min. The main preparation method used in the experiment is hydrolysis. The main raw material is sodium borohydride, and the reaction temperature is 30 °C. In this experiment, in order to improve the hydrogen storage performance of HPSB hydrogen storage material, Co–B and Sm2O3 were introduced as catalysts during the preparation of HPSB. The results show that the amount of Sm2O3 and the ratio of Sm2O3 to Co–B have obvious influence on the hydrogen storage performance of HPSB. In addition, according to the results of SEM analysis, the amount of Sm2O3 and the ratio of Sm2O3 to Co–B also have obvious effects on the microstructure of HPSB hydrogen storage materials. The sample with a doping amount of 4 wt% and a ratio of Sm2O3 to Co–B of 4:6 can release 2.17 wt% H2.