The development of highly efficient bifunctional electrocatalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is crucial for improving the efficiency of overall water splitting, but still remains challenging issue. Herein, 3D self-supported Fe-doped Ni 2 P nanosheet arrays are synthesized on Ni foam by hydrothermal method followed by in situ phosphorization, which serve as bifunctional electrocatalysts for overall water splitting. The as-synthesized (Ni 0.33 Fe 0.67 ) 2 P with moderate Fe doping shows an outstanding OER performance, which only requires an overpotential of ≈230 mV to reach 50 mA cm −2 and is more efficient than the other Fe incorporated Ni 2 P electrodes. In addition, the (Ni 0.33 Fe 0.67 ) 2 P exhibits excellent activity toward HER with a small overpotential of ≈214 mV to reach 50 mA cm −2 . Furthermore, an alkaline electrolyzer is measured using (Ni 0.33 Fe 0.67 ) 2 P electrodes as cathode and anode, respectively, which requires cell voltage of 1.49 V to reach 10 mA cm −2 as well as shows excellent stability with good nanoarray construction. Such good performance is attributed to the high intrinsic activity and superaerophobic surface property.Herein, we fabricated self-supported Fe-doped Ni 2 P nanosheet arrays on the Ni foam by simple hydrothermal method and in situ phosphorization. The performance of Fe-doped Ni 2 P nanosheet arrays as bifunctional catalysts toward overall water splitting depends strongly on the Fe doping ratio in the Ni 2 P. The optimized Fe doping of Ni 2 P [(Ni 0.33 Fe 0.67 ) 2 P] showed excellent HER activity with an overpotential of ≈214 mV to reach 50 mA cm −2 and superior OER performance with a lower overpotential of ≈230 mV to reach 50 mA cm −2 , outperforming the commercial Ir/C. As expected, the electrolyzer using Ni 2 P nanosheet arrays with 31.7% Fe doping as both anode and cathode electrodes for catalyzing overall water splitting exhibited the best performance, obtaining a current density of 10 mA cm −2 at 1.49 V, better than the integration of commercial Pt/C and Ir/C electrodes.