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Inspired by the hard and soft acids and bases principle, we present a modular and hierarchical strategy for the synthesis of aluminum\u2010based mechanically interlocked molecules (AlMIMs) assembled from four synergistic components. Aluminum ions generate robust macrocyclic frameworks through coordination with aromatic carboxylates, while adaptive nitrogen\u2010donor ligands, in concert with structure\u2010directing copper ions, promote axle threading and govern structural dimensionality. This approach creates a full structural library, from discrete [2]\u2010 and [3]rotaxanes to extended polyrotaxane networks, demonstrating broad versatility. Within the spatially confined macrocyclic cavity, copper ions preferentially adopt a stable linear coordination geometry while remaining conformationally flexible outside the cavity to accommodate diverse coordination modes and aggregation states. This dual behavior cooperatively facilitates highly ordered assembly. Notably, the resulting AlMIMs exhibit remarkably enhanced third\u2010order nonlinear optical responses, highlighting emergent properties arising from mechanical interlocking. This work underscores the power of merging coordination chemistry with supramolecular design, transcending conventional static paradigms by revealing how metal ion coordination can be dynamically modulated within precisely engineered supramolecular environments.<\/jats:p>","DOI":"10.1002\/anie.8876257","type":"journal-article","created":{"date-parts":[[2026,5,11]],"date-time":"2026-05-11T07:41:14Z","timestamp":1778485274000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Threading an Aluminum Molecular Ring Onto a Chemically Growing Copper\u2010Directed Polyrotaxane"],"prefix":"10.1002","volume":"65","author":[{"given":"Lin","family":"Geng","sequence":"first","affiliation":[{"name":"State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fuzhou Fujian P. R. 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