Enzyme‐Inspired Hydrogen‐Bonded Organic Frameworks for Synergistic Capture, Detection, and Degradation of Nerve Agent Simulants

FDU‐HOF‐5, an enzyme‐inspired hydrogen‐bonded framework, enables targeted capture, real‐time visual alert, and detoxification of nerve agent simulants through biomimetic sites and multivalent interactions. Integrable into protective gear, it pioneers on‐site threat monitoring strategies for persistent neurotoxic hazards, advancing smart, responsive materials in public safety. Abstract Nerve agents (NAs), a class of highly toxic organophosphorus (OP) compounds, pose a significant threat to global security. The development of integrated protective materials that can simultaneously capture airborne OPs, detect, and degrade them remains a formidable challenge. Inspired by lipase's specific binding to OPs, a biomimetic hydrogen‐bonded organic framework (HOF) is developed, FDU‐HOF‐5. It achieves highly efficient and selective adsorption of a sarin simulant, diethyl chlorophosphate (DCP), by combining size exclusion with molecular recognition via specific N─P bond formation, effectively distinguishing DCP from various OP analogues. Upon adsorption, the material responds within 5 s, enabling bimodal identification via a visual color change (yellow to red) and a fluorescence signal (99.7% quenching, 75 nm redshift). The adsorbed DCP is then self‐drivenly hydrolyzed into non‐toxic products by environmental moisture, achieving 91.5% degradation efficiency. Utilizing the solution processability of HOFs, functional textiles that show an immediate color change upon DCP exposure are produced. This work establishes a rational design strategy for multifunctional HOF systems that synergistically integrate capture, detection, and degradation for effective threat mitigation. FDU-HOF-5, an enzyme-inspired hydrogen-bonded framework, enables targeted capture, real-time visual alert, and detoxification of nerve agent simulants through biomimetic sites and multivalent interactions. Integrable into protective gear, it pioneers on-site threat monitoring strategies for persistent neurotoxic hazards, advancing smart, responsive materials in public safety. Abstract Nerve agents (NAs), a class of highly toxic organophosphorus (OP) compounds, pose a significant threat to global security. The development of integrated protective materials that can simultaneously capture airborne OPs, detect, and degrade them remains a formidable challenge. Inspired by lipase's specific binding to OPs, a biomimetic hydrogen-bonded organic framework (HOF) is developed, FDU-HOF-5. It achieves highly efficient and selective adsorption of a sarin simulant, diethyl chlorophosphate (DCP), by combining size exclusion with molecular recognition via specific N─P bond formation, effectively distinguishing DCP from various OP analogues. Upon adsorption, the material responds within 5 s, enabling bimodal identification via a visual color change (yellow to red) and a fluorescence signal (99.7% quenching, 75 nm redshift). The adsorbed DCP is then self-drivenly hydrolyzed into non-toxic products by environmental moisture, achieving 91.5% degradation efficiency. Utilizing the solution processability of HOFs, functional textiles that show an immediate color change upon DCP exposure are produced. This work establishes a rational design strategy for multifunctional HOF systems that synergistically integrate capture, detection, and degradation for effective threat mitigation. Advanced Science, EarlyView.