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Here, we report a crown\u2013ether\u2013directed lattice assembly that integrates [HfCl\n                    <jats:sub>6<\/jats:sub>\n                    ]\n                    <jats:sup>2\u2012<\/jats:sup>\n                    \/[ZrCl\n                    <jats:sub>6<\/jats:sub>\n                    ]\n                    <jats:sup>2\u2012<\/jats:sup>\n                    octahedra and DB18C6@M(K\n                    <jats:sup>+<\/jats:sup>\n                    \/Rb\n                    <jats:sup>+<\/jats:sup>\n                    ) supramolecular, yielding four unknown organic\u2013inorganic hybrid Hf\/Zr halides. Notably, (DB18C6@K)\n                    <jats:sub>2<\/jats:sub>\n                    (CH\n                    <jats:sub>3<\/jats:sub>\n                    CN)\n                    <jats:sub>2<\/jats:sub>\n                    HfCl\n                    <jats:sub>6<\/jats:sub>\n                    achieves an exceptional room\u2010temperature phosphorescence (RTP) quantum yield (\u03a6\n                    <jats:sub>p<\/jats:sub>\n                    ) of 54.43%, a long lifetime of 0.8 s, and a visually discernible afterglow persisting up to 6 s. Moreover, these materials exhibit excitation\u2013dependent multicolor emission, producing green and blue\u2013white outputs under 302 and 365\u00a0nm irradiation, respectively. This unique multimodal luminescence originates from the synergistic interplay between the balanced soft\u2010rigid lattice provided by the crown\u2010ether framework and heavy\n                    <jats:bold>\u2013<\/jats:bold>\n                    atom Hf\/Zr centers, which facilitates intersystem crossing, enabling both efficient RTP and tunable multichannel pathways. It has been confirmed by the high\u2013pressure synchrotron angle\u2013dispersive x\u2013ray diffraction and Raman results. Overall, this work establishes a heavy\u2013atom\u2013based structural mediation which may offer a generalizable route to high\u2010efficiency, multichannel, and stimuli\u2010responsive RTP materials.\n                  <\/jats:p>","DOI":"10.1002\/anie.2208146","type":"journal-article","created":{"date-parts":[[2026,10,10]],"date-time":"2026-10-10T15:37:08Z","timestamp":1791646628000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Structural Softness\u2013Rigidity Mediation Enables Multicolor Emission and Long\u2010Lived Phosphorescence in Hf\/Zr Halides"],"prefix":"10.1002","author":[{"given":"Yan","family":"Yang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Advanced Fiber Materials College of Materials Science and Engineering Donghua University  Shanghai P. R. 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