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The development of bifunctional electrocatalysts with high catalytic activity and cyclic stability is an effective method for electrocatalytic water splitting. Herein, a promising hydroxide/oxide Co(OH)₂/α-NiMoO₄ NWs/CC heterostructure with nanoflowers decorating the nanowires was fabricated on a carbon cloth (CC) substrate via hydrothermal and calcination methods. In contrast to one-dimensional nanomaterials, the interfaces of Co(OH)₂ nanoflowers and α-NiMoO₄ nanowires on CC provide more active sites for electrocatalytic reactions; therefore, they exhibit obviously enhanced electrocatalytic activities in overall water splitting. Specifically, the Co(OH)₂/α-NiMoO₄ NWs/CC electrodes exhibit an overpotential of 183.01 mV for hydrogen evolution reaction (HER) and of 170.26 mV for oxygen evolution reactions (OER) at the current density of 10 mA cm⁻² in 1.0 M KOH. Moreover, the electrocatalytic oxygen evolution reaction (OER) activity of the Co(OH)₂/α-NiMoO₄ NWs/CC electrocatalyst was enhanced after long-term stability tests.