Nonmetallic High‐Entropy‐Engineered Nanocarbons for Advanced ORR Electrocatalysis

Abstract High‐entropy materials are poised to revolutionize materials science and industrial applications due to their design flexibility, peculiar performance, and broad applicability. In this study, we present a proof‐of‐concept high‐entropy engineered nanocarbon (HENC) co‐doped with five nonmetal elements (B, F, P, S, and N), synthesized via in situ polymerization modification of ZIF‐8 followed by pyrolysis. The HENC exhibits outstanding performance as a nonmetal electrocatalyst for the oxygen reduction reaction (ORR), with activity on par with benchmark Pt/C electrocatalysts and superior cyclic stability. Simulations and all‐site calculations reveal that the synergistic effects of abundant heteroatoms and increased system entropy facilitate the formation of *O 2 species, with N, P, and S acting as the key active elements, while co‐doping with B and F further enhances stability. Notably, HENCs have been validated as cathode catalysts in zinc–air batteries, achieving an impressive peak power density of 604 mW cm −2 and demonstrating long‐term stability over a 16‐day period, outpacing the commercial Pt/C catalyst (542 mW cm −2 ). This work not only enriches the concept of high entropy and advances the understanding of high‐entropy materials but also opens a new avenue for the development of high‐performance low‐cost catalysts.