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Herein, we identify lateral coordination\u2010site blocking as a structural bottleneck in one\u2010dimensional (1D) lead hybrids and demonstrate a lateral\u2010site unblocking strategy to overcome this restriction. Using a model pair, (C\n                    <jats:sub>12<\/jats:sub>\n                    H\n                    <jats:sub>8<\/jats:sub>\n                    N\n                    <jats:sub>2<\/jats:sub>\n                    )Pb(H\n                    <jats:sub>2<\/jats:sub>\n                    PO\n                    <jats:sub>3<\/jats:sub>\n                    )\n                    <jats:sub>2<\/jats:sub>\n                    (PNPP) and (C\n                    <jats:sub>12<\/jats:sub>\n                    H\n                    <jats:sub>8<\/jats:sub>\n                    N\n                    <jats:sub>2<\/jats:sub>\n                    )PbCl\n                    <jats:sub>2<\/jats:sub>\n                    (PNPC), we reveal that the side\u2010occupying H\n                    <jats:sub>2<\/jats:sub>\n                    PO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    linkers enforce a sparse, single\u2010sided hanging mode of phenanthroline (phen) ligands. In contrast, the introduction of compact bridging Cl\n                    <jats:sup>\u2212<\/jats:sup>\n                    ions preserves the 1D Pb\u2010based backbone while releasing the lateral coordination space, thereby enabling a bilateral, tightly interleaved organization of the phen\n                    <jats:italic>\u03c0<\/jats:italic>\n                    \u2010chromophores. This structural switch induces a contraction of the interchain spacing and decreases the interchromophore separation from 6.79 \u00c5 in PNPP to 3.36 \u00c5 in PNPC, resulting in close\n                    <jats:italic>\u03c0<\/jats:italic>\n                    \u2013\n                    <jats:italic>\u03c0<\/jats:italic>\n                    stacking in PNPC and enhanced spatial accumulation of the Pb\u2010centered and\n                    <jats:italic>\u03c0<\/jats:italic>\n                    \u2010conjugated polarizability anisotropy tensors. Consequently, PNPC exhibits an exceptional birefringence of \u0394\n                    <jats:italic>n<\/jats:italic>\n                    = 0.82 at 546\u00a0nm, establishing a record\u2010high value among all reported Pb\u2010based crystalline materials. This work highlights lateral\u2010site accessibility as a decisive structural parameter for regulating lattice\u2010scale polarization alignment, providing a design paradigm for next\u2010generation miniaturized visible\u2010to\u2010near\u2010infrared polarizers.\n                  <\/jats:p>","DOI":"10.1002\/anie.7867481","type":"journal-article","created":{"date-parts":[[2026,8,7]],"date-time":"2026-08-07T13:16:14Z","timestamp":1786108574000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Lateral\u2010Site Unblocking Enables Bilateral\n                    <i>\u03c0<\/i>\n                    \u2010Chromophore Organization for Giant Birefringence in One\u2010Dimensional Lead Hybrids"],"prefix":"10.1002","volume":"65","author":[{"given":"Yuxin","family":"Yan","sequence":"first","affiliation":[{"name":"College of Chemistry and Materials Science Sichuan Normal University  Chengdu People's Republic of China"},{"name":"College of Chemistry Sichuan University  Chengdu People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yingzi","family":"Zhang","sequence":"additional","affiliation":[{"name":"College of Chemistry and Materials Science Sichuan Normal University  Chengdu People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Liyi","family":"Zhang","sequence":"additional","affiliation":[{"name":"College of Chemistry and Materials Science Sichuan Normal University  Chengdu People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ling","family":"Huang","sequence":"additional","affiliation":[{"name":"College of Chemistry and Materials Science Sichuan Normal University  Chengdu People's Republic of 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