rechargeable batteries, the key to realizing high performance lies in electrode materials. [7][8][9][10][11][12] However, traditional electrode materials, such as graphite, conductive polymers (CPs), and transition metal oxides, have the drawbacks of low capacitance, high cost, and poor stability, which are far from enough to satisfy the requirements of high energy density, high capacity rate, and long cycle life. In comparison with rechargeable batteries, SCs have the advantages of long cycle life, fast chargeÀdischarging capability, and high-power density, but their wide adhibition is impeded by the low-rate capability and inferior energy density. For fuel cells, their overall efficiency is severely hampered via the sluggish oxygen reduction reaction (ORR). Similarly, in the electrochemical energy conversion system of water splitting, the two half reactions (at the anode: oxygen evolution reaction (OER), at the cathode: hydrogen evolution reaction (HER)) require an excess of driving force to overcome resistance such as activation energy barriers from the electrode/electrolyte and solution contact interfaces. Therefore, efficient electrocatalysts are urgently needed to optimize the efficiency of specific applications. To date, the commercial electrocatalysts for ORR, HER, and OER are mainly precious metal-based materials (e.g., Pt-based materials for HER and ORR and Ru-/Ir-based materials for OER). Nonetheless, their expensive cost and inferior durability greatly restrict the widespread practical applications in renewable energy technologies. [13] In view of these limitations, it is urgently needed to develop costeffective electroactive materials with high activity and long-term durability, being challenges.MetalÀorganic frameworks (MOFs), which are known as porous coordination polymers (PCPs), are a class of crystalline porous materials assembled by inorganic nodes (clusters/metal ions) and organic ligands through coordination bonds. [14][15][16][17][18][19][20] Up to now, MOFs, as functional materials, have received extensive attention in multiple advanced technology adhibition, such as separation, [21,22] drug delivery, [23][24][25] sensing, [26,27] gas adsorption, [28,29] catalysis, [30,31] and energy storage. [32][33][34][35][36][37][38][39] As MOFs are constructed by two main components, the structure can be easily adjusted to realize the desired properties for target applications by properly selecting the organic ligands and inorganic nodes. [40][41][42][43][44][45][46][47][48][49] Recently, MOF-based materials have been proved to be more competitive than other porous materials as electroactive materials in electrochemical energy storage and conversion due to their high specific surface areas, huge and clear void structures, and uniform