Tailoring the nanostructure/morphology and chemical composition is important to regulate the electronic configuration of electrocatalysts and thus enhance their performance for water and urea electrolysis. Herein, the nitrogen-doped carbon-decorated tricomponent metal phosphides of FeP₄ nanotube@Ni-Co-P nanocage (NC-FNCP) with unique nested hollow architectures are fabricated by a self-sacrifice template strategy. Benefiting from the multi-component synergy, the modification of nitrogen-doped carbon, and the modulation of nested porous hollow morphology, NC-FNCP facilitates rapid electron/mass transport in water and urea electrolysis. NC-FNCP-based anode shows low potentials of 248 mV and 1.37 V (vs. reversible hydrogen electrode) to attain 10 mA/cm² for oxygen evolution reaction (OER) and urea oxidation reaction (UOR), respectively. In addition, the overall urea electrolysis drives 10 mA/cm² at a comparatively low voltage of 1.52 V (vs. RHE) that is 110 mV lower than that of overall water electrolysis, as well as exhibits excellent stability over 20 h. This work strategizes a multi-shell-structured electrocatalyst with multi-compositions and explores its applications in a sustainable combination of hydrogen production and sewage remediation.