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To enable high\u2010fidelity recognition of such chemically inert targets, we propose a generalizable \u201cSteric\u2010Engineered Thermodynamic Gating\u201d strategy based on disaggregation\u2010induced emission (DIE) mechanism that breaks the intrinsic \u201cstability\u2010sensitivity\u201d deadlock in supramolecular sensing. Distinct from trial\u2010and\u2010error optimization, this approach rationally exploits steric bulk to induce active packing frustration, creating metastable aggregates designed to selectively detect SCs via synergistic non\u2010covalent interactions (e.g., \u03c0\u2013\u03c0 stacking and hydrogen bonding). Functioning as a thermodynamic filter, this assembly remains inert against non\u2010target interferents yet selectively undergoes cooperative disassembly upon binding with specific SCs via multivalent synergy, transforming a quenched \u201coff\u201d state into a robust blue\u2010shifted \u201con\u201d signal. Validating this strategy with EDMB\u2010PINACA, the system exhibits ultrafast response (&lt;1 s) and high sensitivity (LOD 4.7\u00a0\u00b5M); integrated into a 3D\u2010printed portable chip, it enables reliable, false\u2010positive\u2010free screening in authentic samples (e.g., e\u2010liquids, petals) with exceptional immunity to complex matrix interference. This work establishes a methodological blueprint for engineering aggregate metastability to recognize low\u2010reactivity analytes, offering a theoretical foundation for designing intelligent field\u2010deployable optics beyond the limitations of traditional molecular recognition.<\/jats:p>","DOI":"10.1002\/anie.3463809","type":"journal-article","created":{"date-parts":[[2026,5,20]],"date-time":"2026-05-20T10:49:44Z","timestamp":1779274184000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Steric\u2010Engineered Thermodynamic Gating: Metastable Assemblies for Chemical\u2010Class Discrimination of Synthetic Cannabinoids"],"prefix":"10.1002","volume":"65","author":[{"given":"Fengbin","family":"Tao","sequence":"first","affiliation":[{"name":"School of Chemistry and Chemical Engineering Shihezi University  Shihezi 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