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Here, we report a groundbreaking CsAg\n                    <jats:sub>2<\/jats:sub>\n                    I\n                    <jats:sub>3<\/jats:sub>\n                    \/GaN van der Waals (vdWs) heterojunction that uniquely integrates in\u2010plane structural anisotropy, pronounced pyro\u2010phototronic effect, and atomically sharp interface engineering. The CsAg\n                    <jats:sub>2<\/jats:sub>\n                    I\n                    <jats:sub>3<\/jats:sub>\n                    single\u2010crystals, synthesized via chemical vapor deposition, exhibit a wide\u2010bandgap (\u223c3.38\u00a0eV), strong second\u2010order nonlinear response, and remarkable pyroelectricity, overcoming the stability and symmetry limitations of conventional perovskites and inorganic wide\u2010bandgap semiconductors. The CsAg\n                    <jats:sub>2<\/jats:sub>\n                    I\n                    <jats:sub>3<\/jats:sub>\n                    \/GaN device delivers record\u2010breaking performance: an ultralow dark current of 0.3\u00a0pA, high responsivity of 0.28\u00a0A\/W, specific detectivity of 1.7\u00a0 \u00d7 10\n                    <jats:sup>12<\/jats:sup>\n                    Jones, and ultrafast response speeds of 16\/21\u00a0\u00b5s, outperforming most state\u2010of\u2010the\u2010art perovskites and wide\u2010bandgap photodetectors. Crucially, the pyro\u2010phototronic effect amplifies polarization sensitivity, achieving an unprecedented dichroic ratio of 10.5 under bias, the highest reported for all\u2010inorganic perovskite systems and other competitors. The device also demonstrates exceptional operational stability and robust performance in an information\u2010splitting encryption system, validating its real\u2010world applicability. This work establishes a new paradigm for synergizing pyro\u2010phototronics and structural anisotropy in heterostructures, enabling a versatile platform for high\u2010performance, self\u2010powered, polarization\u2010sensitive optoelectronics.\n                  <\/jats:p>","DOI":"10.1002\/advs.74896","type":"journal-article","created":{"date-parts":[[2026,3,18]],"date-time":"2026-03-18T19:22:47Z","timestamp":1773861767000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Synergistic Pyro\u2010Phototronics and Structural Anisotropy in CsAg\n                    <sub>2<\/sub>\n                    I\n                    <sub>3<\/sub>\n                    \/GaN Heterostructures for High\u2010Performance Polarization\u2010Sensitive UV Photodetectors"],"prefix":"10.1002","volume":"13","author":[{"given":"Yalin","family":"Zhai","sequence":"first","affiliation":[{"name":"College of Physics MIIT Key Laboratory of Aerospace Information Sensing and Physics Key Laboratory for Intelligent Nano Materials and Devices Nanjing University of Aeronautics and Astronautics  Nanjing Jiangsu P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Siqi","family":"Wang","sequence":"additional","affiliation":[{"name":"Jilin Key Laboratory of Solid\u2010State Laser Technology and Application School of Physics Changchun University of Science and Technology  Changchun Jilin P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Peng","family":"Guo","sequence":"additional","affiliation":[{"name":"College of Physics MIIT Key Laboratory of Aerospace Information Sensing and Physics Key Laboratory for Intelligent Nano Materials and Devices Nanjing University of Aeronautics and Astronautics  Nanjing Jiangsu P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Songling","family":"Feng","sequence":"additional","affiliation":[{"name":"College of Physics MIIT Key Laboratory of Aerospace Information Sensing and Physics Key Laboratory for Intelligent Nano Materials and Devices Nanjing University of Aeronautics and Astronautics  Nanjing Jiangsu P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Peng","family":"Wan","sequence":"additional","affiliation":[{"name":"College of Physics MIIT Key Laboratory of Aerospace Information Sensing and Physics Key Laboratory for Intelligent Nano Materials and Devices Nanjing University of Aeronautics and Astronautics  Nanjing Jiangsu P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jilong","family":"Tang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of High Power Semiconductor Laser Changchun University of Science and Technology  Changchun Jilin P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Caixia","family":"Kan","sequence":"additional","affiliation":[{"name":"College of Physics MIIT Key Laboratory of Aerospace Information Sensing and Physics Key Laboratory for Intelligent Nano Materials and Devices Nanjing University of Aeronautics and Astronautics  Nanjing Jiangsu P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hui","family":"Li","sequence":"additional","affiliation":[{"name":"Jilin Key Laboratory of Solid\u2010State Laser Technology and Application School of Physics Changchun University of Science and Technology  Changchun Jilin P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Daning","family":"Shi","sequence":"additional","affiliation":[{"name":"College of Physics MIIT Key Laboratory of Aerospace Information Sensing and Physics Key Laboratory for Intelligent Nano Materials and Devices Nanjing University of Aeronautics and Astronautics  Nanjing Jiangsu P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1784-582X","authenticated-orcid":false,"given":"Mingming","family":"Jiang","sequence":"additional","affiliation":[{"name":"College of Physics MIIT Key Laboratory of Aerospace Information Sensing and Physics Key Laboratory for Intelligent Nano Materials and Devices Nanjing University of Aeronautics and Astronautics  Nanjing Jiangsu P. R. 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