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Elaborate design of highly active catalysts from earth-abundant elements is important for the development of water-splitting devices. We have synthesized {2̅ 1 1} high index-faceted Ni12P5 nanoplates and Ni12P5 spherical nanoparticles (SNPs) by the one-step solvothermal method. The Ni12P5 nanoplates show enhanced hydrogen evolution reaction activity with a lower overpotential of −128 mV and a smaller Tafel slope of 60.6 mV dec−1 compared to Ni12P5 SNPs. Stability tests reveal exceptional durability of the catalyst. This study offers an attractive catalytic material for large-scale hydrogen production technology. [ABSTRACT FROM AUTHOR]