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Selectively cracking the inert C\u2500C bonds in polyolefins under mild, co\u2010reactant\u2010free conditions remains a fundamental challenge due to their chemical stability and poor diffusivity. Herein, we report a co\u2010reactant\u2010free strategy for the selective cracking of polyolefin into C\n                    <jats:sub>2<\/jats:sub>\n                    \u2013C\n                    <jats:sub>6<\/jats:sub>\n                    olefins at 240\u00a0\u00b0C under 1\u00a0atm N\n                    <jats:sub>2<\/jats:sub>\n                    , enabled by\n                    <jats:italic>b<\/jats:italic>\n                    \u2010axis\u2010shortened HZSM\u20105 nanosheet zeolites (s\u2010ZSM\u20105) with tailored micropore confinement and acidity. Mechanistic investigations reveal an isomerization\u2013oligomerization\u2013scission (IOS) cycle confined within zeolite micropores, which arises from the synergistic interplay of controlled confinement and diffusion. This dynamic cycle is driven by the preferential diffusion of short\u2010chain olefins, which disrupts local reaction equilibrium and drives continuous cracking. The optimized s\u2010ZSM\u20105 catalyst achieves up to 94.7% low\u2010density polyethylene (LDPE) conversion and 90.0% C\n                    <jats:sub>2<\/jats:sub>\n                    \u2013C\n                    <jats:sub>6<\/jats:sub>\n                    olefin selectivity, while exhibiting exceptional coking resistance and compatibility with diverse post\u2010consumer plastics. These findings establish a novel mechanistic foundation for confined\u2010space effect and offer guiding principles for the rational design of solid catalysts for sustainable plastic upcycling.\n                  <\/jats:p>","DOI":"10.1002\/anie.202525081","type":"journal-article","created":{"date-parts":[[2026,1,21]],"date-time":"2026-01-21T11:30:21Z","timestamp":1768995021000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Mild\u2010Condition Upcycling of Polyolefins Enabled by Micropore Confinement in Zeolites"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0000-5277-4479","authenticated-orcid":false,"given":"Zhuohan","family":"Lin","sequence":"first","affiliation":[{"name":"Key Laboratory for Advanced Materials Feringa Nobel Prize Scientist Joint Research Center School of Chemistry and Molecular Engineering East China University of Science and Technology  Shanghai 200237 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