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Here, a simple, yet efficient approach to improve sodium (Na) storage on these C6\u2010benzene rings within a porous polymeric framework by rationally regulating their steric hindrance is reported. Decreasing intrinsic hindrance affords a significant improvement in redox reaction kinetics within the porous architecture, thereby facilitating the acceptance of Na ions on these functionalized benzene rings and boosting the SIB performance. As a result, the modulate porous framework exhibits an exceptional battery capacity of 376 mAh g<jats:sup>\u22121<\/jats:sup> after 1000 cycles at 1.0 A g<jats:sup>\u22121<\/jats:sup>, which is \u22481.5 times larger than that of the pristine framework. Furthermore, the performance can reach as high as 510 mAh g<jats:sup>\u22121<\/jats:sup> at 0.1 A g<jats:sup>\u22121<\/jats:sup>, comparable to that of the best\u2010performing polymeric electrodes. The simple modulation approach not only enables Na storage modulation on functionalized C6\u2010benzene rings, but also simultaneously provides a means to extend the understanding of the structure\u2010property relationship and facilitate new possibilities for organic SIBs.<\/jats:p>","DOI":"10.1002\/smll.202105927","type":"journal-article","created":{"date-parts":[[2021,12,4]],"date-time":"2021-12-04T12:45:47Z","timestamp":1638621947000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":19,"title":["Regulating Steric Hindrance in Redox\u2010Active Porous Organic Frameworks Achieves Enhanced Sodium Storage Performance"],"prefix":"10.1002","volume":"18","author":[{"given":"Yilin","family":"Shan","sequence":"first","affiliation":[{"name":"Key Laboratory for Ultrafine Materials of Ministry of Education Shanghai Engineering Research Center of Hierarchical Nanomaterials School of Materials Science and Engineering East China University of Science and Technology  Shanghai 200237 China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Yanyan","family":"He","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Engineering School of Chemical Engineering East China University of Science and Technology  Shanghai 200237 China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Na","family":"Yang","sequence":"additional","affiliation":[{"name":"State Key Laboratory for Oxo Synthesis and Selective Oxidation Suzhou Research Institute of Lanzhou Institute of Chemical Physics Chinese Academy of Sciences  Suzhou 215000 China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Xiang","family":"Zhu","sequence":"additional","affiliation":[{"name":"State Key Laboratory for Oxo Synthesis and Selective Oxidation Suzhou Research Institute of Lanzhou Institute of Chemical Physics Chinese Academy of Sciences  Suzhou 215000 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