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Inspired by \u03b2\u2010sheet proteins, where branched side chains act as steric directors to program backbones into interlocked architectures, a side\u2010chain isomerization strategy is proposed to manipulate analogous NoCL networks for constructing planar\u2010structured NIR\u2010II multimodal PTAs. Two isomeric pairs with linear (\n                    <jats:italic>l<\/jats:italic>\n                    \u2010series) and branched (\n                    <jats:italic>b<\/jats:italic>\n                    \u2010series) alkyl side\u2010chains are synthesized. Crystallographic analysis reveals that the\n                    <jats:italic>b<\/jats:italic>\n                    \u2010series, driven by directional S\u00b7\u00b7\u00b7O\/F interactions, adopts a fully planar conformation stabilized by a synergistic dual NoCL network, whereas\n                    <jats:italic>l<\/jats:italic>\n                    \u2010series exhibits twisted conformations. Theoretical calculation and femtosecond transient absorption spectra confirm the dual NoCL network effectively narrows the energy gap and optimizes excited\u2010state energy dissipation pathway, resulting in comprehensive enhancement in phototheranostic performance including superior ROS generation, higher NIR\u2010II brightness and excellent photothermal properties compared to\n                    <jats:italic>l<\/jats:italic>\n                    \u2010series NPs. Notably, the exceptional performance of\n                    <jats:italic>b<\/jats:italic>\n                    \u20103CPFIC NPs enables it to serve as an ideal candidate in multimodal NIR\u2010II phototheranostics of tumors. This work establishes a novel design paradigm for multifunctional PTAs and elucidates aggregate\u2010level structure\u2013property relationships.\n                  <\/jats:p>","DOI":"10.1002\/advs.76688","type":"journal-article","created":{"date-parts":[[2026,7,24]],"date-time":"2026-07-24T09:57:21Z","timestamp":1784887041000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Engineering Synergistic Intra\u2010\/Intermolecular Conformational Locking via Side\u2010Chain Branching: A \u03b2\u2010Sheet\u2010Inspired Strategy for Planar NIR\u2010II Phototheranostic Aggregates"],"prefix":"10.1002","volume":"13","author":[{"given":"Cheng","family":"Lu","sequence":"first","affiliation":[{"name":"Department of Chemistry Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction Division of Life Science and State Key Laboratory of Molecular Neuroscience The Hong Kong University of Science and Technology  Kowloon Hong Kong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qian","family":"Jia","sequence":"additional","affiliation":[{"name":"Lab of Molecular Imaging and Translational Medicine (MITM) Engineering Research Center of Molecular and Neuro Imaging Ministry of Education School of Life Science and Technology Xidian University &amp; International Joint Research Center for Advanced Medical Imaging and Intelligent Diagnosis and Treatment  Xi'an Shaanxi China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1446-408X","authenticated-orcid":false,"given":"Bo","family":"Wu","sequence":"additional","affiliation":[{"name":"School of Environmental and Chemical Engineering Wuyi University  Jiangmen Guangdong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0455-9146","authenticated-orcid":false,"given":"Chao","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Chemistry The Hong Kong University of Science and Technology  Kowloon Hong Kong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6866-3877","authenticated-orcid":false,"given":"Ryan T. K.","family":"Kwok","sequence":"additional","affiliation":[{"name":"Department of Chemistry Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction Division of Life Science and State Key Laboratory of Molecular Neuroscience The Hong Kong University of Science and Technology  Kowloon Hong Kong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6555-5099","authenticated-orcid":false,"given":"Tie\u2010Gen","family":"Chen","sequence":"additional","affiliation":[{"name":"Zhongshan Institute for Drug Discovery Shanghai Institute of Materia Medica Chinese Academy of Sciences  Zhongshan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2470-1077","authenticated-orcid":false,"given":"Jianwei","family":"Sun","sequence":"additional","affiliation":[{"name":"Department of Chemistry The Hong Kong University of Science and Technology  Kowloon Hong Kong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5536-0439","authenticated-orcid":false,"given":"Zheng","family":"Zhao","sequence":"additional","affiliation":[{"name":"Guangdong Basic Research Center of Excellence for Aggregate Science School of Science and Engineering The Chinese University of Hong Kong (Shenzhen)  Shenzhen Guangdong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9480-615X","authenticated-orcid":false,"given":"Teng\u2010Teng","family":"Chen","sequence":"additional","affiliation":[{"name":"Department of Chemistry The Hong Kong University of Science and Technology  Kowloon Hong Kong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9388-149X","authenticated-orcid":false,"given":"Zhongliang","family":"Wang","sequence":"additional","affiliation":[{"name":"Lab of Molecular Imaging and Translational Medicine (MITM) Engineering Research Center of Molecular and Neuro Imaging Ministry of Education School of Life Science and Technology Xidian University &amp; International Joint Research Center for Advanced Medical Imaging and Intelligent Diagnosis and Treatment  Xi'an Shaanxi China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jacky W. 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