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This invention provides a self-supporting one-dimensional nanorod array composite material, its preparation method, and its application, belonging to the field of clean energy harvesting technology. The preparation method provided by this invention includes the following steps: mixing soluble nickel salt, soluble molybdate, and water, and carrying out a hydrothermal reaction to obtain a NiMo precursor; heat-treating the NiMo precursor and a modifier under a protective atmosphere to obtain the self-supporting one-dimensional nanorod array composite material. Experimental results show that the composite material prepared by the method provided by this invention has excellent electrocatalytic water splitting activity and operational stability, and photo-assisted synthesis further enhances the electrocatalytic water splitting activity of the composite material, making it applicable to solar-driven electrocatalytic water splitting.