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Here, a time\u2010resolved physically unclonable function (TR\u2010PUF) system is established, transforming optical authentication from static pattern recognition to high\u2010dimensional temporal encoding. Central to this approach, boron\u2010based room\u2010temperature phosphorescent (RTP) materials are developed via covalent coupling with coumarin derivatives using a solvent\u2010free strategy that is readily scalable to kilogram\u2010level production, exhibiting a maximum phosphorescence lifetime of over 2 s, an ultralong afterglow visible for up to 30 s, and color\u2010tunable emission. The formation of rigid B\u2010O\u2010C linkages spatially isolates emissive centers, suppressing energy transfer and preserving temporally independent decay channels\u2013an essential prerequisite for high\u2010entropy time\u2010resolved encoding. Randomly embedding these multi\u2010emissive RTP units into a polymer matrix forms a complex encryption structure that enables a dual\u2010entropy encoding mechanism with both spectral and temporal dimensions, generating dynamic time keys for authentication. Moreover, we propose a matched time\u2010gated authentication framework that achieves &gt;99% identification accuracy within 1.2 s while exhibiting resistance against the tested generative machine\u2010learning attacks. This work proposes a practical materials platform and a time\u2010gated authentication strategy, offering a scalable technological path for the development of dynamic optical encryption tags.<\/jats:p>","DOI":"10.1002\/adma.75237","type":"journal-article","created":{"date-parts":[[2026,10,12]],"date-time":"2026-10-12T09:58:16Z","timestamp":1791799096000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Time\u2010Resolved Physically Unclonable Functions Enabled by Solvent\u2010Free Scalable Boron\u2010Based Ultralong Phosphorescent Systems for Machine\u2010Learning\u2010Resilient Optical Encryption"],"prefix":"10.1002","author":[{"given":"Changsong","family":"Xu","sequence":"first","affiliation":[{"name":"School of Chemical Engineering and Light Industry Guangdong University of Technology  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Daxiang","family":"Shi","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering and Light Industry Guangdong University of Technology  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Guoyi","family":"Pan","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering and Light Industry Guangdong University of Technology  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ru\u2010Jia","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering and Light Industry Guangdong University of Technology  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiankang","family":"Qin","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering and Light Industry Guangdong University of Technology  Guangzhou P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4715-9839","authenticated-orcid":false,"given":"Wenjing","family":"Lin","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering and Light Industry Guangdong University of Technology  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3788-3516","authenticated-orcid":false,"given":"Wen\u2010Cheng","family":"Chen","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering and Light Industry Guangdong University of Technology  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4802-0812","authenticated-orcid":false,"given":"Xiaofeng","family":"Lin","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering and Light Industry Guangdong University of Technology  Guangzhou P. R. 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