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This capability to externally control neuronal signaling via optical stimuli has provided profound insights into brain function and established a versatile strategy for engineering bio\u2010inspired information processing. Herein, a designable van der Waals (vdW) crystal has been demonstrated for device\u2010scale neuronal cell mimicking. The structural similarity between ion\u2010channel in biological membranes and layered vdW lattices is realized with nano\u2010crystallization. As the sequential transition from carrier transport dominance to ion transport dominance reveals the dynamic control over synaptic weight updates. Optoelectric synaptic plasticity in designable vdW crystal (long\u2010term potentiation and depression, paired\u2010pulse facilitation, and a tunable short\u2010term to long\u2010term memory transition) were conclusively observed and correlates with photo\u2010induced carrier trapping and ionic migration. Furthermore, learning\u2010forgetting\u2010relearning cycles achieve 34.7% increased retention efficiency compared to bulk ReSe\n                    <jats:sub>2<\/jats:sub>\n                    . Functional demonstrations in edge detection and CIFAR\u201010 image recognition confirm the synaptic plasticity into system\u2010level neuromorphic computation, with a recognition accuracy of 96.24%. In conclusion, we envision that designable vdW artificial crystal will provide the versatile advances for 3D stackable neuromorphic vision architectures.\n                  <\/jats:p>","DOI":"10.1002\/adma.73595","type":"journal-article","created":{"date-parts":[[2026,6,3]],"date-time":"2026-06-03T07:17:07Z","timestamp":1780471027000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Designable van der Waals Crystal for Artificial Neuronal Cell Mimicking"],"prefix":"10.1002","volume":"38","author":[{"given":"Jinhyoung","family":"Lee","sequence":"first","affiliation":[{"name":"School of Mechanical Engineering Sungkyunkwan University (SKKU)  Suwon\u2010si Gyeonggi\u2010do South Korea"},{"name":"Center For Quantum Nanoscience Institute For Basic Science (IBS)  Seoul South 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