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Memristors with superior computing ability are among the most promising computing blocks. However, conventional vertical Metal\/Resistive layer\/Metal (V\u2010MRM) memristors tend to generate intense electric fields, suffer from limited sensory response, inflexible, and rigid functional modes, as well as long\u2010standing variability and overshoot issues. Here, we present an unconventional two\u2010terminal quasi\u2010vertical (QV) van der Waals heterostructure (vdWH) memristor as opto\u2010reconfigurable hardware. Unlike the V\u2010MRM memristor with a strong, rigid vertical electric field, this QV\u2010vdWH memristor realizes a significantly softened, tunable electric field, enabling parametric configurable and wavelength\u2010dependent reconfigurable modes across nonvolatile\/volatile memory, neurons, synapses, and optical perception. Moreover, the light\u2010memristive switching\u2010vdWH coupling triggers a super\u2010additive synergistic enhancement of memristive performance (&gt; 100\u2010fold) and photoresponse (&gt; 3000\u2010fold). Meanwhile, the long\u2010standing variability and overshoot issues are overcome, yielding ultra\u2010uniform memristive behavior with even a single\u2010valued distribution. Leveraging the opto\u2010reconfigurability, high\u2010accuracy object tracking, and human motion recognition (\u223c96.8%) are successfully performed. Breaking through the inherent functional limitation of the conventional V\u2010MRM memristive structure, the QV\u2010vdWH memristor provides a flexible, opto\u2010reconfigurable hardware platform for emerging computing paradigms, and AI applications.<\/jats:p>","DOI":"10.1002\/adma.75098","type":"journal-article","created":{"date-parts":[[2026,9,21]],"date-time":"2026-09-21T10:47:31Z","timestamp":1789987651000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["A Single Quasi\u2010Vertical van der Waals Heterostructure Memristor as Opto\u2010Reconfigurable Artificial Intelligence Hardware"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0006-9357-2412","authenticated-orcid":false,"given":"Yesheng","family":"Li","sequence":"first","affiliation":[{"name":"School of Physics and Technology Wuhan University  Wuhan China"},{"name":"Suzhou Institute of Wuhan University  Suzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-7602-0321","authenticated-orcid":false,"given":"Changxu","family":"Yin","sequence":"additional","affiliation":[{"name":"School of Physics and Technology Wuhan University  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4909-7790","authenticated-orcid":false,"given":"Xiaolin","family":"Zhang","sequence":"additional","affiliation":[{"name":"School of Physics and Technology Wuhan University  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Gaoli","family":"Luo","sequence":"additional","affiliation":[{"name":"School of Physics and Technology Wuhan University  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0009-5470-3549","authenticated-orcid":false,"given":"Yi","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Physics and Technology Wuhan University  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenkai","family":"Zhou","sequence":"additional","affiliation":[{"name":"School of Physics and Technology Wuhan University  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1041-1906","authenticated-orcid":false,"given":"Yao","family":"Xiong","sequence":"additional","affiliation":[{"name":"School of Physics and Mechanics Wuhan University of Technology Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5998-5225","authenticated-orcid":false,"given":"Jun","family":"He","sequence":"additional","affiliation":[{"name":"School of Physics and Technology Wuhan University  Wuhan China"},{"name":"Wuhan Institute of Quantum Technology  Wuhan China"},{"name":"Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences  Beijing 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