The hydrogen-storage purification is studied with hydrogen-storage alloy, LaNi5, as the purification agent, and its design and optimization method is established based on the integration of hydrogen network. Relationships among the hydrogen-saving capacity of unit hydrogen-storage material, the required weight of hydrogen-storage material, hydrogen-storage time, and purification feed purity are deduced and used in the design and optimization. An optimization procedure is proposed to identify the optimal purification feed, the maximum hydrogen utility savings, the amount of required hydrogen-storage material, and the hydrogen absorption time. The hydrogen networks of two refineries are optimized by the proposed method. With the designed hydrogen-storage purification units, their hydrogen utility consumption can be reduced by 23.11% and 44.69%, respectively. In both cases, the optimal purification hydrogen feed purity, the optimal hydrogen recovery and the consumption of LaNi5 hydrogen-storage material are identified; the economic performance of the hydrogen-storage purification is compared with that of pressure swing adsorption.