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Here, we report the first synthesis and characterization of a well\u2010defined CPP triple\u2010decker molecule, denoted as CPP\u2010TD, which maintains a persistent cylindrical geometry at room temperature. This structure is efficiently constructed via a concise, stereoselective cyclocondensation reaction. X\u2010ray crystallographic analysis confirms a rigid\n                    <jats:italic>cis\u2013cis<\/jats:italic>\n                    cylindrical conformation in the solid state, a geometry that is retained in solution as evidenced by spectroscopic studies. The observed shape persistency arises from attractive van der Waals (vdW) interactions between adjacent CPP layers. Owing to its rigid cylindrical architecture and alternating donor\u2013acceptor constitution, CPP\u2010TD exhibits distinctive optical properties and demonstrates strong binding affinity toward fullerene C\n                    <jats:sub>70<\/jats:sub>\n                    , forming a tight 1:2 host\u2013guest complex.\n                  <\/jats:p>","DOI":"10.1002\/anie.8876064","type":"journal-article","created":{"date-parts":[[2026,3,18]],"date-time":"2026-03-18T14:10:41Z","timestamp":1773843041000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Cylindrical Cycloparaphenylene Triple\u2010Decker"],"prefix":"10.1002","volume":"65","author":[{"given":"Zhuofan","family":"Xu","sequence":"first","affiliation":[{"name":"Department of Chemistry, Institute of Molecular Plus Tianjin University  Tianjin P. R. 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