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Herein, two isomorphic ionic MOFs (IMOF\u2010DMF and IMOF\u2010DEF) are constructed via in situ decarbonylation of DMF\/DEF, leveraging guest\u2010ion size to regulate ligand conjugation through modulation of pyridine ring dihedral angles. IMOF\u2010DEF exhibits superior room\u2010temperature phosphorescence (RTP) and temperature\u2010dependent behavior. Mechanistic studies reveal that reduced conjugation enhances intersystem crossing (ISC) by strengthening spin\u2010orbit coupling while minimizing the singlet\u2010triplet energy gap (\u0394E\n                    <jats:sub>st<\/jats:sub>\n                    ). Furthermore, a dual\u2010parameter anti\u2010counterfeiting platform and flexible PVA hydrogel films enable advanced information encryption through temperature\/time\u2010resolved signals and triple\u2010state lifetime encoding. This work establishes ligand conjugation engineering as a key strategy for tailoring MOF photophysics, linking molecular design to optoelectronic applications and security technologies.\n                  <\/jats:p>","DOI":"10.1002\/advs.202509013","type":"journal-article","created":{"date-parts":[[2025,7,12]],"date-time":"2025-07-12T14:43:21Z","timestamp":1752331401000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["Molecular Engineering of Ionic Metal\u2010Organic Frameworks via Ligand Conjugation Modulation for Tailored Phosphorescence and Multilevel Encryption"],"prefix":"10.1002","volume":"12","author":[{"given":"Qi","family":"Wu","sequence":"first","affiliation":[{"name":"Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education College of Chemistry &amp; Materials Science Northwest University  Xi'an 710127 P. R. 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