Cobalt-based　catalysts　have　emerged　as　promising　substitutes　for　Pt-　and　Cr-based　propane　dehydrogenation　(PDH)　catalysts.　However,　controlling　the　distribution　of　Co　species　and　achieving　stable　active　centers　remains　challenging.　Here,　we　report　that　reaction-driven　reconstruction　of　metallic　cobalt　(Co0)　species　within　pure　silica　MFI　zeolite　(S-1)　into　CoOx　clusters　within　silanol　nests　during　PDH　yields　efficient　and　durable　performance.　Atomically　dispersed　CoOx　clusters　exhibit　exceptional　durability　and　high　propylene　space-time　yield　(STY),　maintaining　an　ultrahigh　propylene　STY　of　17.2 mmolC3H6 gcat−1 h−1　for　over　260 h　under　industrially　relevant　conditions,　surpassing　previous　cobalt-based　PDH　catalysts.　Moreover,　the　catalyst　operates　stably　at　520 °C　for　170 h　with　near-equilibrium　propane　conversions.　Comprehensive　characterizations　indicate　the　dynamic　evolution　process　from　the　silanol　nests　effectively　capturing　and　stabilizing　Co0　species　within　S-1　zeolite,　thereby　promoting　the　dynamic　formation　of　CoOx　clusters　during　the　PDH　process.　We　also　demonstrate　that　stable　Co─O　active　centers　formed　by　this　unique　anchoring　strategy　improve　catalyst　stability　by　suppressing　coke　formation　and　promoting　efficient　propane　dehydrogenation.　©　2025　Wiley-VCH　GmbH.