LAUSR

Optoelectronic synapses combining optical‐sensing and synaptic functions are playing an increasingly vital role in the neuromorphic computing systems development, which can efficiently process visual information and complex recognition, memory, and learning. Metal halides are considered promising candidates for synaptic devices due to their excellent optoelectronic properties. However, the toxicity of lead and the further development of device functions are the recognized problems at present. Herein, a flexible optoelectronic synapses system based on high‐quality lead‐free Cs3Bi2I9 nanocrystals is demonstrated, in which the carrier confinement caused by the band mismatching between the Cs3Bi2I9 and the organic semiconductor layer provides the possibility to simulate synaptic behaviors. The synaptic functions including long/short‐term memory and learning‐forgetting‐relearning are demonstrated in this device and visual perception, visual memory, and color recognition functions are successfully implemented. Additionally, the flexible device exhibits excellent robustness and can realize imaging of light distribution under curved hemispheres similar to the human eye. Finally, through the simulation based on an artificial neural network algorithm, the device successfully realizes the high‐precision recognition of handwritten digital images and possesses a strong fault tolerant capability even in bending states. These results are expected to drive the practical progress of metal halide for neuromorphic computing.