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Hydrogen is one of the most promising green energy alternatives due to its high gravimetric energy density, zero-carbon emissions, and other advantages. In this work, a CoFeBP micro-flower (MF) electrocatalyst is fabricated as an advanced water-splitting electrocatalyst by a hydrothermal approach for hydrogen production with the highly efficient hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). The fabrication process of the CoFeBP MF electrocatalyst is systematically optimized by thorough investigations on various hydrothermal synthesis and post-annealing parameters. The best optimized CoFeBP MF electrode demonstrates HER/OER overpotentials of 20 mV and 219 mV at 20 mA/cm2. The CoFeBP MFs also exhibit a low 2-electrode (2-E) cell voltage of 1.60 V at 50 mA/cm2, which is comparable to the benchmark electrodes of Pt/C and RuO2. The CoFeBP MFs demonstrate excellent 2-E stability of over 100 h operation under harsh industrial operational conditions at 60 °C in 6 M KOH at a high current density of 1000 mA/cm2. The flower-like morphology can offer a largely increased electrochemical active surface area (ECSA), and systematic post-annealing can lead to improved crystallinity in CoFeBP MFs.