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Self‐supported electrodes comprising carbon fiber paper (CP) integrated with bifunctional nickel phosphide (Ni‐P) electrocatalysts are fabricated by electrodeposition of Ni on functionalized CP, followed by a convenient one‐step phosphorization treatment in phosphorus vapor at 500 °C. The as‐fabricated CP@Ni‐P electrode exhibits excellent electrocatalytic performance toward hydrogen evolution in both acidic and alkaline solutions, with only small overpotentials of 162 and 250 mV, respectively, attaining a cathodic current density of 100 mA cm⁻². Furthermore, the CP@Ni‐P electrode also exhibits superior catalytic performance toward oxygen evolution reaction (OER). An exceptionally high OER current of 50.4 mA cm⁻² is achieved at an overpotential of 0.3 V in 1.0 m KOH. The electrode can sustain 10 mA cm⁻² for 180 h with only negligible degradation, showing outstanding durability. Detailed microstructural …