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Here, we develop a rational molecular design strategy to isolate pressure\u2010induced single\u2010molecule deformation as the key factor of PIEE in 0D copper iodide hybrids. By systematically tuning the alkyl\u2010chain length of quaternary phosphonium cations, we construct a series of single crystals, (EtPPh\n                    <jats:sub>3<\/jats:sub>\n                    )\n                    <jats:sub>2<\/jats:sub>\n                    Cu\n                    <jats:sub>2<\/jats:sub>\n                    I\n                    <jats:sub>4<\/jats:sub>\n                    , (PrPPh\n                    <jats:sub>3<\/jats:sub>\n                    )\n                    <jats:sub>2<\/jats:sub>\n                    Cu\n                    <jats:sub>2<\/jats:sub>\n                    I\n                    <jats:sub>4<\/jats:sub>\n                    , and (BuPPh\n                    <jats:sub>3<\/jats:sub>\n                    )\n                    <jats:sub>2<\/jats:sub>\n                    Cu\n                    <jats:sub>2<\/jats:sub>\n                    I\n                    <jats:sub>4<\/jats:sub>\n                    , which exhibit distinct crystal\u2010packing modes and distortions while preserving a [Cu\n                    <jats:sub>2<\/jats:sub>\n                    I\n                    <jats:sub>4<\/jats:sub>\n                    ] emissive core. In this work, \u201csingle\u2010molecule deformation\u201d refers to the pressure\u2010induced geometric evolution of an individual discrete [Cu\n                    <jats:sub>2<\/jats:sub>\n                    I\n                    <jats:sub>4<\/jats:sub>\n                    ]\n                    <jats:sup>2\u2212<\/jats:sup>\n                    emissive unit within the crystal lattice. Pressure\u2010dependent structural, spectroscopic, kinetic, and theoretical analyses show that crystal packing and intermolecular interactions govern pressure transmission and suppress nonradiative relaxation, while deformation of the initially pre\u2010distorted [Cu\n                    <jats:sub>2<\/jats:sub>\n                    I\n                    <jats:sub>4<\/jats:sub>\n                    ]\n                    <jats:sup>2\u2212<\/jats:sup>\n                    unit in (PrPPh\n                    <jats:sub>3<\/jats:sub>\n                    )\n                    <jats:sub>2<\/jats:sub>\n                    Cu\n                    <jats:sub>2<\/jats:sub>\n                    I\n                    <jats:sub>4<\/jats:sub>\n                    drives excited\u2010state reconfiguration and activates radiative decay. Consequently, its photoluminescence (PL) intensity reaches 208\u2010fold the ambient\u2010pressure value at 2.6\u00a0GPa, and the absolute photoluminescence quantum yield (PLQY) rises from 0.68% to 84.59%. These results identify single\u2010molecule deformation as the predominant structural origin of its high PIEE. Moreover, we demonstrate a power\u2010free preload\u2010sensing gasket and multilevel pressure\u2010encoded optical encryption, underscoring the application potential of pressure\u2010responsive luminescence.\n                  <\/jats:p>","DOI":"10.1002\/anie.1615351","type":"journal-article","created":{"date-parts":[[2026,9,21]],"date-time":"2026-09-21T07:39:41Z","timestamp":1789976381000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Pressure\u2010Induced Single\u2010Molecule Deformation Enables 208\u2010Fold Photoluminescence\u2010Intensity Enhancement in Zero\u2010Dimensional Copper Iodide Hybrids"],"prefix":"10.1002","author":[{"given":"Shuqi","family":"Zhang","sequence":"first","affiliation":[{"name":"Key Laboratory of Functional Inorganic Material Chemistry (Ministry of Education) &amp; School of Chemistry and Material Science Heilongjiang University  Harbin P. R. 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