As excellent materials, high-entropy alloys have excellent mechanical properties, wear resistance, oxidation resistance, corrosion resistance, physical properties, and radiation resistance. This work presents the design and preparation of a novel high-entropy alloy based on the BCC structure, added with lanthanum, and shows excellent catalytic performance in the hydrolysis of ammonia borane. The high-entropy alloy catalyst being able to catalyse the complete release of hydrogen in 1.3 min at 323 K, and the value of turnover frequency (TOF) value as high as 93.96 min −1 . The value of the apparent activation energy (Ea) can reach 26.98 kJ/mol. It retains good catalytic performance after 10 cycles of catalytic hydrogen production from equivalent amounts of boron ammonia at 303 K. In this work, a new strategy is presented to improve the performance of transition group high-entropy alloys and the potential energy and environmental benefits of these alloys are demonstrated.