Ir, and Ru have been regarded as state-ofthe-art electrocatalysts. Nevertheless, the processing stability and cost-effectiveness of noble metal-based catalysts are still the major concerns in the development of industrial water electrolysis. [4] Correspondingly, tremendous efforts have been devoted to the search for stable and costeffective alternatives, e.g., transition-metal alloys, [5] oxides, [6,7] sulfides, [8,9] selenides, [10] etc. It is not until recent years that transition metal phosphides (TMPs) were reported to exhibit significant potentials as high-performance, bifunctional electrocatalysts for both half-cell reactions in overall water splitting, which is an obvious plus for further cost optimization. [11-13] In general, bulky cheap metal-based materials can hardly reach the high activity compared with the benchmark noble-metal catalysts. This drawback, however, can be potentially compensated through morphology modulation and electronic structure tuning. The former is generally achieved by the constructions of micro-/ nanoarchitectures to expose more active sites. While the latter can be realized through dopant incorporation to optimize the binding strength of reaction intermediates on active sites. [2,11] Consequently, many reported high-performance electrocatalysts possess porous nanostructures composed with bimetallic or trimetallic compounds, such as CoNi hydroxide@hydroxysulfide core-shell heterostructure, [14] Co-Fe-P nanotubes, [15] Cr-doped