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PEOs with various end groups were threaded into pillar[5]arene rings in a mixture of water and methanol to afford pseudopolyrotaxanes. Corresponding polyrotaxanes were also constructed by capping COOH‐terminated pseudopolyrotaxanes with bulky amines, in which multiple hydrogen bonds involving the pillar[5]arene OH groups were critically important to prevent dethreading. The number of threaded ring components could be rationally controlled in these materials, providing a simple and versatile method to tune the mechanical and thermal properties. Specifically, a polyrotaxane with a high‐molecular‐weight axle became elastic upon heating above the melting point of PEOs and exhibited temperature‐dependent shape memory property because of the topological confinement and crosslinked hydrogen bonds.</jats:p>"}]}],"creator":[{"@id":"https://cir.nii.ac.jp/crid/1380009142738989185","@type":"Researcher","foaf:name":[{"@value":"Kenichi Kato"}],"jpcoar:affiliationName":[{"@value":"Department of Synthetic Chemistry and Biological Chemistry Graduate School of Engineering Kyoto University  Nishikyo-ku Kyoto 6158510 Japan"}]},{"@id":"https://cir.nii.ac.jp/crid/1380009142738989060","@type":"Researcher","foaf:name":[{"@value":"Katsuto Onishi"}],"jpcoar:affiliationName":[{"@value":"Department of Synthetic Chemistry and Biological Chemistry Graduate School of Engineering Kyoto University  Nishikyo-ku Kyoto 6158510 Japan"}]},{"@id":"https://cir.nii.ac.jp/crid/1380009142738989062","@type":"Researcher","foaf:name":[{"@value":"Koki 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