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Designing and optimizing structure is an effective method to enhance electrocatalytic performance of transition metal-based catalysts. In this work, an innovative nanostructured electrode, consisted of peapod-like Ni 2 P@N-doped carbon nanorods array coating on carbon fiber (CF@p-Ni 2 P@NC), is devised and synthesized. The N-doped carbon layer is crucial for maintaining the peapod-like nanostructure, which allows for multi-channel electrolyte transport and gas product release. And the carbon layer coating Ni 2 P nanoparticles also enhance electrical conductivity and stability, thus ensuring fast electron transport from/to active sites and the long-term stability of catalyst during urea oxidation reaction (UOR)/hydrogen evolution reaction (HER). Benefit from the reasonable structure, CF@p-Ni 2 P@NC present perfect performance with getting 100 mA cm−2 at potential/overpotential of 1.417/0.194 V for UOR/HER in 1.0 M KOH containing 0.5 M urea. In addition, the overall urea-electrolysis system using CF@p-Ni 2 P@NC bifunctional electrode only requires 1.590 V to obtain 100 mA cm−2. Novel peapod-like Ni 2 P@N-doped carbon nanorods array on carbon fiber is prepared and exhibits perfect catalytic activity toward both UOR and HER in urea-assisted electrolytic water splitting. [Display omitted] • Peapod-like Ni 2 P@N-doped carbon nanorods array on CF is designed and synthesized. • The CF@p-Ni 2 P@NC exhibits perfect catalytic activity toward both UOR and HER. • The superior performance is ascribed to the peapod-like nanorods array structure. [ABSTRACT FROM AUTHOR]