Oxygen Vacancy‐Engineered High‐Entropy Oxide Nanozymes for Spatiotemporal Cascading Antifouling in Marine Environments

ABSTRACT The catalytic versatility and compositional tunability of oxidative attack‐based nanozymes offer a promising strategy for marine antifouling, yet their performance is often constrained by insufficient active‐site accessibility, transient catalytic intermediates and restricted diffusion. Inspired by haloperoxidases (HPOs) in marine organisms, this study reports oxygen vacancy (V o )‐enriched high‐entropy oxides (V o ‐HEO) as multifunctional nanozymes to address these challenges. The entropy‐stabilized multicomponent lattice, synergistically coupled with abundant V o sites, reconfigures electronic structures and diversifies catalytic pathways, enabling efficient HPO‐mimetic generation of hypobromous acid (HOBr), which is a selective and long‐lived biocide (half‐life > 36 days) capable of disrupting bacterial quorum sensing (QS) signals and oxidizing key biomolecules. By further integrating persistent HOBr with highly reactive hydroxyl radicals, V o ‐HEO establishes a spatiotemporally cascading protective regime at the substrate interface, combining long‐range QS suppression in the bulk phase with rapid oxidative eradication at the nano‐biological interface, ultimately reducing bacterial adhesion by 90%. Microbiological characterization and metagenomic sequencing analyses further verify that V o ‐HEO systematically collapses the coordination of microbial communication and energy metabolism across temporal and spatial scales. Collectively, this work demonstrates intelligent regulation of marine microecology and establishes a paradigm for adaptive antifouling design.