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Abstract An amorphous Ni nanoparticles‐loaded ZnO nanowire array is controllably constructed on stainless steel mesh through combined electrodeposition and hydrothermal reaction. Its nano‐arrayed structure not only provides a platform to achieve stable and good dispersion of Ni nanoparticles, but also helps improve their ability to adsorb 4‐nitrophenolate ions and to capture hydrogen radicals, thereby accelerating the hydrogen transfer from metal hydride complex to 4‐nitrophenol. Benefiting from the abovementioned unique features, it outperforms most Ni‐based catalysts. While a 30‐s re‐electrodeposition of Ni can provide it extra 150 min of high catalytic activity towards the reduction of waste 4‐nitrophenol to valuable 4‐aminophenol, further demonstrating its outstanding reusability. The highly general methodology reported here paves the way to economically and effectively synthesize various other metal nanoparticles‐loaded ZnO nanowire arrays on different conductive substrates, which not only enrich the nanowire‐arrayed catalysts, but also significantly promote their practical utilizations in a wide range of environment‐related fields.