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Here, we first report a crystallography\u2010guided design of intrinsically dynamic MOFs that overcome this longstanding challenge. A crystallography\u2013catalysis feedback loop with dimensionality and ligand\u2010flexibility tuning built a homologous Zn\u2010MOF series, revealing intrinsically dynamic, layer\u2010pillared\n                    <jats:bold>Zn\u2010Bpe<\/jats:bold>\n                    as the optimal catalyst. Mechanistic studies with a ligand\u2010substituted rigid analogue, host\u2010guest binding, density functional theory (DFT), and ab initio molecular dynamics (AIMD) reveal an adaptive catalytic mechanism where guests induce in situ framework dynamics, enhancing the diffusion of the substrates and the activity of the catalytic center. This dynamicity enables efficient and selective multicomponent couplings, exhibiting broad substrate tolerance and functional group compatibility, including a tandem domino Petasis reaction. Our findings establish intrinsic dynamicity as a generalizable design principle in MOF catalysis, balancing accessibility, selectivity, and structural integrity in complex transformations.\n                  <\/jats:p>","DOI":"10.1002\/anie.7413214","type":"journal-article","created":{"date-parts":[[2026,5,14]],"date-time":"2026-05-14T09:18:16Z","timestamp":1778750296000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Crystal Engineering of Intrinsic Dynamicity in Metal\u2010Organic Frameworks for Adaptive Multicomponent Catalysis"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-9737-687X","authenticated-orcid":false,"given":"Xu","family":"Jia","sequence":"first","affiliation":[{"name":"Department of Chemistry KU Leuven  Leuven 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