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Herein, an interfacial lattice\u2010distortion engineering strategy is proposed by selectively substituting phenylethyl ammonium (PEA) cations with 4\u2010chlorophenylethylammonium (Cl\u2010PEA) at perovskite heterointerfaces. This substitution induces beneficial octahedral distortions, boosting hole transport efficiency in few\u2010layer 2D perovskites by 26%. When integrated with MoS\n                    <jats:sub>2<\/jats:sub>\n                    \/WSe\n                    <jats:sub>2<\/jats:sub>\n                    heterostructures, the optimized van der Waals contact and enhanced energy\u2010level alignment yield a high\u2010performance photodetection, including a responsivity of 2.7 \u00d7 10\n                    <jats:sup>4<\/jats:sup>\n                    A\/W, a detectivity up to 5.26 \u00d7 10\n                    <jats:sup>14<\/jats:sup>\n                    \u00a0Jones, and an exceptionally low noise equivalent power of 0.42\u00a0fW\u00a0Hz\n                    <jats:sup>\u22121\/2<\/jats:sup>\n                    . Notably, the device operates self\u2010powered at incident power densities as low as 0.54\u00a0\u00b5W\u00a0cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , enabling real\u2010time, on\u2010chip image processing even under dim\u2010light conditions. This functionality is further utilized for noise reduction in traffic\u2010light images prior to object detection with YOLOv11 network, establishing a direct bridge between device\u2010level photodetection and machine\u2010learning\u2010driven recognition. This interfacial lattice distortion engineering paradigm in van der Waals\u2010contacted 2D devices opens new avenues for designing ultrasensitive, low\u2010noise, and functionally integrated optoelectronic devices.\n                  <\/jats:p>","DOI":"10.1002\/adma.202507636","type":"journal-article","created":{"date-parts":[[2025,6,13]],"date-time":"2025-06-13T01:36:54Z","timestamp":1749778614000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["Ultra\u2010Sensitive Optoelectronics Enabled by Atomically Tailored Interfaces Engineering for Advanced Perceptual Imaging"],"prefix":"10.1002","volume":"37","author":[{"given":"Ziqiao","family":"Wu","sequence":"first","affiliation":[{"name":"Institute of New Energy Technology College of Physics &amp; Optoelectronic Engineering Jinan University  Guangzhou 510632 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