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Designable van der Waals crystal has been demonstrated for device?scale neuronal cell mimicking. The structural similarity between ion?channel in biological membranes and layered vdW lattices is realized with nano?crystallization via Ar + H2S plasma sulfurization. As the sequential transition from intralayer migration to coupled intra?/interlayer migration reveals the dynamic control of synaptic weight updates. Optoelectronic synaptic plasticity in designable vdW were conclusively observed and correlates with photo?induced carrier trapping and ionic migration. Furthermore, learning?forgetting?relearning cycles achieves 34.7 % increased retention efficiency compared to bulk ReSe2. Functional demonstrations in edge detection and CIFAR?10 image recognition confirm the synaptic plasticity into system?level neuromorphic computation, with a recognition accuracy of 96.24%. In conclusion, our designable vdW crystal will offer the generalizable platform for next?generation 3D integrated neuromorphic device and edge?computing AI hardware.ABSTRACTOptogenetics employs light to regulate neuronal activity with exceptional spatiotemporal precision, thereby enabling the direct modulation of learning and memory processes in the human brain. 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?inspired information processing. Herein, a designable van der Waals (vdW) crystal has been demonstrated for device?scale neuronal cell mimicking. The structural similarity between ion?channel in biological membranes and layered vdW lattices is realized with nano?crystallization. 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?term potentiation and depression, paired?pulse facilitation, and a tunable short?term to long?term memory transition) were conclusively observed and correlates with photo?induced carrier trapping and ionic migration. Furthermore, learning?forgetting?relearning cycles achieve 34.7% increased retention efficiency compared to bulk ReSe2. Functional demonstrations in edge detection and CIFAR?10 image recognition confirm the synaptic plasticity into system?level 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.