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While MOC structures are uniquely and precisely predetermined by the metal coordination number and ligand configuration, tailoring MOCs to further modulate the size, shape, and chemical environment of the cavities has become intensively studied for a more efficient and adaptive molecular binding. Herein, we report self\u2010expanding MOCs that exhibit remarkable structural variations in cage size and flexibility while maintaining their topology. A cyclic ligand with an oligomeric chain tethering the two benzene rings of stilbene was designed and mixed with Rh<jats:sup>II<\/jats:sup> ions to obtain the parent MOCs. These MOCs were successfully transformed into expanded MOCs via the selective cleavage of the double bond in stilbene. The expanded MOCs could effectively trap multidentate <jats:italic>N<\/jats:italic>\u2010donor molecules in their enlarged cavity, in contrast to the original MOCs with a narrow cavity. As the direct synthesis of expanded MOCs is impractical because of the entropically disfavored structures, self\u2010expansion using ring\u2010openable ligands is a promising approach that allows precision engineering and the production of functional MOCs that would otherwise be inaccessible.<\/jats:p>","DOI":"10.1002\/anie.202404155","type":"journal-article","created":{"date-parts":[[2024,3,8]],"date-time":"2024-03-08T03:16:40Z","timestamp":1709867800000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["Fabrication of Self\u2010Expanding Metal\u2013Organic Cages Using a Ring\u2010Openable Ligand"],"prefix":"10.1002","volume":"63","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-6475-0383","authenticated-orcid":false,"given":"Ami","family":"Nishijima","sequence":"first","affiliation":[{"name":"Department of Applied Chemistry Graduate School of Engineering The University of Tokyo  7-3-1 Hongo, Bunkyo-ku 113-8656 Tokyo Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0009-2727-9551","authenticated-orcid":false,"given":"Yuto","family":"Osugi","sequence":"additional","affiliation":[{"name":"Department of Applied Chemistry Graduate School of Engineering The University of Tokyo  7-3-1 Hongo, Bunkyo-ku 113-8656 Tokyo Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1357-3196","authenticated-orcid":false,"given":"Takashi","family":"Uemura","sequence":"additional","affiliation":[{"name":"Department of Applied Chemistry Graduate School of Engineering The University of Tokyo  7-3-1 Hongo, Bunkyo-ku 113-8656 Tokyo Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2024,3,22]]},"reference":[{"key":"e_1_2_3_1_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.200805340"},{"key":"e_1_2_3_2_1","doi-asserted-by":"publisher","DOI":"10.1039\/C5CS00861A"},{"key":"e_1_2_3_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41565-020-0652-2"},{"key":"e_1_2_3_4_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41570-020-00246-1"},{"key":"e_1_2_3_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/ar970224v"},{"key":"e_1_2_3_6_1","doi-asserted-by":"publisher","DOI":"10.1039\/b008684n"},{"key":"e_1_2_3_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/cr200077m"},{"key":"e_1_2_3_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201000380"},{"key":"e_1_2_3_9_1","doi-asserted-by":"publisher","DOI":"10.1038\/nchem.2452"},{"key":"e_1_2_3_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201611875"},{"key":"e_1_2_3_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201805244"},{"key":"e_1_2_3_12_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.8b01701"},{"key":"e_1_2_3_13_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-018-06872-0"},{"key":"e_1_2_3_14_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202000045"},{"key":"e_1_2_3_15_1","doi-asserted-by":"publisher","DOI":"10.1039\/C6CS00907G"},{"key":"e_1_2_3_16_1","doi-asserted-by":"publisher","DOI":"10.1039\/C8CS00978C"},{"key":"e_1_2_3_17_1","doi-asserted-by":"publisher","DOI":"10.1002\/cplu.202000279"},{"key":"e_1_2_3_18_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41570-022-00380-y"},{"key":"e_1_2_3_19_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2017.11.015"},{"key":"e_1_2_3_20_1","doi-asserted-by":"publisher","DOI":"10.1038\/nchem.803"},{"key":"e_1_2_3_21_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201207373"},{"key":"e_1_2_3_22_1","doi-asserted-by":"publisher","DOI":"10.1039\/D0CS00801J"},{"key":"e_1_2_3_23_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41557-023-01387-8"},{"key":"e_1_2_3_24_1","doi-asserted-by":"publisher","DOI":"10.1038\/ncomms15356"},{"key":"e_1_2_3_25_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemmater.7b04128"},{"key":"e_1_2_3_26_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.8b09682"},{"key":"e_1_2_3_27_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.7b12916"},{"key":"e_1_2_3_28_1","doi-asserted-by":"publisher","DOI":"10.1039\/D0TA08009H"},{"key":"e_1_2_3_29_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202111228"},{"key":"e_1_2_3_30_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202310354"},{"key":"e_1_2_3_31_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.inorgchem.6b02091"},{"key":"e_1_2_3_32_1","unstructured":"Deposition numbers 2314934 (for1) and 2314935 (for1\u2032+tpt) contain the supplementary crystallographic data for this paper. 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