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However, translating molecular\u2010level photoswitching into sequence\u2010dependent macroscopic outputs in the solid state remains a formidable challenge. In this study, we report a supramolecular strategy that integrates guanyl hydrazone switches into hydrogen\u2010bonded organic frameworks (HOFs) to overcome this limitation. A tetrasulfonate\u2010substituted tetraphenylethylene anion (\n                    <jats:bold>\n                      TPE\n                      <jats:sup>4<\/jats:sup>\n                      <jats:sup>\u2212<\/jats:sup>\n                    <\/jats:bold>\n                    ) is employed as the host scaffold, while guanyl hydrazone (\n                    <jats:bold>G2<\/jats:bold>\n                    ) functions as the photoresponsive guest, affording a functional framework through cooperative assembly. This system leverages a reversible crystalline\u2013amorphous phase transformation, triggered by acid\u2013base stimuli, to gate the solid\u2010state photoisomerization of\n                    <jats:bold>G2<\/jats:bold>\n                    . Upon activation, the configurational switching of\n                    <jats:bold>G2<\/jats:bold>\n                    induces a cascade reorganization of the\n                    <jats:bold>\n                      TPE\n                      <jats:sup>4<\/jats:sup>\n                      <jats:sup>\u2212<\/jats:sup>\n                    <\/jats:bold>\n                    packing motifs, leading to pronounced and sequence\u2010dependent modulation of both fluorescence and macroscopic coloration. In addition, the applicability of this system in information encryption has been demonstrated. This work expands the design paradigm of hydrazone\u2010based photoswitches in the solid state and provides a supramolecular strategy for constructing intelligent optical materials with high information density and enhanced security.\n                  <\/jats:p>","DOI":"10.1002\/anie.7471326","type":"journal-article","created":{"date-parts":[[2026,9,23]],"date-time":"2026-09-23T03:42:43Z","timestamp":1790134963000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Ammonia\u2010Gated Guanyl Hydrazone Photoisomerization Enables Sequential Solid\u2010State Optical Response in Hydrogen\u2010Bonded Organic Frameworks"],"prefix":"10.1002","author":[{"given":"Weixu","family":"Feng","sequence":"first","affiliation":[{"name":"Xi'an Key Laboratory of Hybrid Luminescent Materials and Photonic Device School of Chemistry and Chemical engineering Northwestern Polytechnical University  Xi'an 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9964-680X","authenticated-orcid":false,"given":"Yan","family":"Zhao","sequence":"additional","affiliation":[{"name":"Xi'an Key Laboratory of Hybrid Luminescent Materials and Photonic Device School of Chemistry and Chemical engineering Northwestern Polytechnical University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2159-4181","authenticated-orcid":false,"given":"Wei","family":"Tian","sequence":"additional","affiliation":[{"name":"Xi'an Key Laboratory of Hybrid Luminescent Materials and Photonic Device School of Chemistry and Chemical engineering Northwestern Polytechnical University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7432-2385","authenticated-orcid":false,"given":"Hongxia","family":"Yan","sequence":"additional","affiliation":[{"name":"Xi'an Key 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