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In this work, a targeted structural design strategy centered on introducing cation\u2010ordered sites and optimizing hydrogen bond networks was proposed and executed, which successfully aligns the polarized [NO\n                    <jats:sub>3<\/jats:sub>\n                    ] and [SO\n                    <jats:sub>3<\/jats:sub>\n                    NH\n                    <jats:sub>2<\/jats:sub>\n                    ] groups in parallel and achieves synergistic enhancement of optical anisotropy. Guided by this strategy, four new UV nitrate sulfamates were synthesized. Among them, the calculated birefringence of K\n                    <jats:sub>2<\/jats:sub>\n                    (NO\n                    <jats:sub>3<\/jats:sub>\n                    )(SO\n                    <jats:sub>3<\/jats:sub>\n                    NH\n                    <jats:sub>2<\/jats:sub>\n                    ) (0.122 at 546\u00a0nm), Rb\n                    <jats:sub>2<\/jats:sub>\n                    (NO\n                    <jats:sub>3<\/jats:sub>\n                    )(SO\n                    <jats:sub>3<\/jats:sub>\n                    NH\n                    <jats:sub>2<\/jats:sub>\n                    ) (0.116 at 546\u00a0nm) and K\n                    <jats:sub>0.5<\/jats:sub>\n                    (NH\n                    <jats:sub>4<\/jats:sub>\n                    )\n                    <jats:sub>1.5<\/jats:sub>\n                    (NO\n                    <jats:sub>3<\/jats:sub>\n                    )(SO\n                    <jats:sub>3<\/jats:sub>\n                    NH\n                    <jats:sub>2<\/jats:sub>\n                    ) (0.126 at 546\u00a0nm) display about 2.7\u2010, 2.5\u2010 and 2.8\u2010fold higher than that of Rb\n                    <jats:sub>1.7<\/jats:sub>\n                    (NH\n                    <jats:sub>4<\/jats:sub>\n                    )\n                    <jats:sub>0.3<\/jats:sub>\n                    (NO\n                    <jats:sub>3<\/jats:sub>\n                    )(SO\n                    <jats:sub>3<\/jats:sub>\n                    NH\n                    <jats:sub>2<\/jats:sub>\n                    ) (0.045 at 546\u00a0nm), with these values exceeding all the birefringence reported to date for metal sulfamates, nitrate sulfamates and co\u2010crystal. More importantly, this study elucidates how the regulation of cation\u2010occupied cooperative hydrogen bond networks drives structural transformations and clarifies the underlying origins of birefringence and its enhancement. These findings provide valuable insights and guidance for the rational design of short\u2010wavelength UV birefringent materials.\n                  <\/jats:p>","DOI":"10.1002\/smll.73327","type":"journal-article","created":{"date-parts":[[2026,4,10]],"date-time":"2026-04-10T06:49:07Z","timestamp":1775803747000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Synergistic Enhancement of Optical Anisotropy in Nitrate Sulfamate for UV Applications: Role of Functional Group Alignment and Hydrogen Bond Network"],"prefix":"10.1002","volume":"22","author":[{"given":"Xiaotian","family":"Ma","sequence":"first","affiliation":[{"name":"Research Center for Crystal Materials CAS Key Laboratory of Functional Materials and Devices for Special Environmental Conditions Xinjiang Key Laboratory of Functional Crystal Materials Xinjiang Technical Institute of Physics &amp; Chemistry Chinese Academy of Sciences  Urumqi 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