Abstract: | The functionalization with phosphotriesterase of poly(isoprene‐b‐styrene‐b‐4‐vinylpyridine)‐based nanoporous membranes fabricated by self‐assembly and nonsolvent induced phase separation (SNIPS) is shown to enable dynamically responsive membranes capable of substrate‐specific and localized gating response. Integration of the SNIPS process with macroporous nylon support layers yields mechanically robust textile‐type films with high moisture vapor transport rates that display rapid and local order‐of‐magnitude modulation of permeability. The simplicity of the fabrication process that is compatible with large‐area fabrication along with the versatility and efficacy of enzyme reactivity offers intriguing opportunities for engineered biomimetic materials that are tailored to respond to a complex range of external parameters, providing sensing, protection, and remediation capabilities. |