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In a hydrogen-storage alloy which is a high-entropy alloy having a molecular formula of CouFevMnwTixVyZrz, the hydrogen-storage alloy is an alloy free from rare-earth elements and having a stable single C14 Laves phase structure. The hydrogen-storage alloy has a high capacity of absorbing and releasing hydrogen under ambient temperature and pressure and a high hydrogen-storage capacity at room temperature, so that the hydrogen-storage alloy can be used extensively in the fields of hydrogen storage, heat storage, heat pump, hydrogen purification, isotope separation, secondary battery and fuel cell without producing harmful polluted gases, and the hydrogen-storage alloy has high potential for the development of a green energy source.