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However, establishing precise structure\u2013property relationships remains a fundamental challenge due to the complex, non-equilibrium dynamic processes\u2014such as transient solvation, competing hydrogen-bonding networks, and mesoscopic phase separation\u2014that occur during dissolution and gelation. Traditional static and post-mortem characterizations fail to capture these spatiotemporally dynamic behaviors, creating a critical knowledge gap. To overcome this bottleneck, the integration of real-time in situ\/operando characterization techniques with multiscale computational simulations has established a novel, synergistic paradigm. This review comprehensively synthesizes recent advances in decoding the multiscale architectures of cellulose ionogels. We systematically analyze how molecular-scale calculations and time-resolved vibrational\/electronic spectroscopies reveal interfacial solvation mechanisms and dynamic bond cleavage\/reconstruction. We further evaluate how mesoscopic scattering, nanomechanical mapping, and rheological tools resolve network topology and structural heterogeneity. By bridging these multiscale diagnostics with macroscopic transport and mechanics, the dynamic coupling\/decoupling mechanisms governing ionic conductivity, mechanical toughness, and thermal stability are critically decoded. Finally, key technical bottlenecks and future trajectories\u2014including physics-informed machine learning, operando multi-field coupling probes, and AI-driven inverse material design\u2014are outlined, providing theoretical guidelines and technical blueprints for next-generation sustainable ionogels.<\/jats:p>","DOI":"10.3390\/gels12090837","type":"journal-article","created":{"date-parts":[[2026,9,14]],"date-time":"2026-09-14T13:05:26Z","timestamp":1789391126000},"page":"837","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Cellulose Ionogels: Unraveling Structure\u2013Property Relationships Through Multiscale In-Situ Characterization and Theoretical Modeling"],"prefix":"10.3390","volume":"12","author":[{"ORCID":"https:\/\/orcid.org\/0009-0001-1851-964X","authenticated-orcid":false,"given":"Jia","family":"Wei","sequence":"first","affiliation":[{"name":"State Key Laboratory of Water Engineering Ecology and Environment in Arid Area, School of Eco-Environmental and Chemical Engineering, Xi\u2019an University of Technology, Xi\u2019an 710048, China"},{"name":"School of Chemical Engineering, University of Chinese Academy of Sciences, Beijing 100049, China"},{"name":"Zhengzhou Institute of Emerging Industrial Technology, Zhengzhou 450000, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ziyan","family":"He","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Water Engineering Ecology and Environment in Arid Area, School of Eco-Environmental and Chemical Engineering, Xi\u2019an University of Technology, Xi\u2019an 710048, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jingtao","family":"Ruan","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Water Engineering Ecology and Environment in Arid Area, School of Eco-Environmental and Chemical Engineering, Xi\u2019an University of Technology, Xi\u2019an 710048, China"},{"name":"Zhengzhou Institute of Emerging Industrial Technology, Zhengzhou 450000, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junjie","family":"Ou","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Water Engineering Ecology and Environment in Arid Area, School of Eco-Environmental and Chemical Engineering, Xi\u2019an University of Technology, Xi\u2019an 710048, China"},{"name":"Zhengzhou Institute of Emerging Industrial Technology, Zhengzhou 450000, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wen","family":"Zhang","sequence":"additional","affiliation":[{"name":"Zhengzhou Institute of Emerging Industrial Technology, Zhengzhou 450000, China"},{"name":"School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bin","family":"Tan","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering, University of Chinese Academy of Sciences, Beijing 100049, China"},{"name":"Zhengzhou Institute of Emerging Industrial Technology, Zhengzhou 450000, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaoheng","family":"He","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Water Engineering Ecology and Environment in Arid Area, School of Eco-Environmental and Chemical Engineering, Xi\u2019an University of Technology, Xi\u2019an 710048, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhen","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Water Engineering Ecology and Environment in Arid Area, School of Eco-Environmental and Chemical Engineering, Xi\u2019an University of Technology, Xi\u2019an 710048, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yufei","family":"Tang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Water Engineering Ecology and Environment in Arid Area, School of Eco-Environmental and Chemical Engineering, Xi\u2019an University of Technology, Xi\u2019an 710048, China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"1968","published-online":{"date-parts":[[2026,9,12]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","unstructured":"Lim, K.J.H., Lu, W., Ng, S.W.L., Gao, M., and Ho, G.W. 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