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Herein, we propose a programmable linker regioisomerization strategy within zeolitic imidazolate frameworks (ZIFs) to modulate their stimulus\u2010responsive structural flexibility, thereby significantly enhancing SF\n                    <jats:sub>6<\/jats:sub>\n                    capture efficiency from nitrogen (N\n                    <jats:sub>2<\/jats:sub>\n                    ) streams. Simultaneous regioisomerization of the methyl group in ZIF\u20108 and the aldehyde group in ZIF\u201090 on the imidazolate linkers yields ZIF\u201094, which exhibits a rare guest\u2010induced reversible framework deformation upon SF\n                    <jats:sub>6<\/jats:sub>\n                    adsorption. This behavior confers an enzyme\u2010like induced\u2010fit recognition mechanism for SF\n                    <jats:sub>6<\/jats:sub>\n                    molecules, strengthening host\u2013guest interactions. As a result, ZIF\u201094 achieves a high SF\n                    <jats:sub>6<\/jats:sub>\n                    adsorption capacity of 1.97\u00a0mmol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    and an ultrahigh SF\n                    <jats:sub>6<\/jats:sub>\n                    stacking density of 1438.69\u00a0mg cm\n                    <jats:sup>\u22123<\/jats:sup>\n                    at 298\u00a0K and 0.1\u00a0bar, along with dramatically enhanced SF\n                    <jats:sub>6<\/jats:sub>\n                    \/N\n                    <jats:sub>2<\/jats:sub>\n                    selectivities over ZIF\u20108 and ZIF\u201090. In situ experiments and theoretical analyses reveal that the SF\n                    <jats:sub>6<\/jats:sub>\n                    \u2010induced structural flexibility of ZIF\u201094 allows the framework to dynamically adjust and optimize its cage structure to match gas molecules, thus leading to significantly reinforced SF\n                    <jats:sub>6<\/jats:sub>\n                    \/N\n                    <jats:sub>2<\/jats:sub>\n                    separation performance. The experimental column breakthrough tests and pressure swing adsorption simulations confirm the practical separation performance for SF\n                    <jats:sub>6<\/jats:sub>\n                    \/N\n                    <jats:sub>2<\/jats:sub>\n                    mixtures in ZIF\u201094. This work offers useful insights for designing flexible adsorbents for gas separation applications.\n                  <\/jats:p>","DOI":"10.1002\/anie.3448513","type":"journal-article","created":{"date-parts":[[2026,9,1]],"date-time":"2026-09-01T10:50:20Z","timestamp":1788259820000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Adaptive Induced\u2010Fit via Engineered Linker Regioisomerization in Biomimetic Zeolitic Imidazolate Frameworks for Boosting SF\n                    <sub>6<\/sub>\n                    \/N\n                    <sub>2<\/sub>\n                    Separation"],"prefix":"10.1002","volume":"65","author":[{"given":"Qiang","family":"Zhang","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering Academy for Advanced Interdisciplinary Studies Nankai University  Tianjin 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