AbstractOptoelectronic synaptic devices integrating light‐perception and signal‐storage functions hold great potential in neuromorphic computing for visual information processing, as well as complex brain‐like learning, memorizing, and reasoning. Herein, the successful growth of MoS2monolayer arrays assisted by gold nanorods guided precursor nucleation is demonstrated. Optical, spectral, and morphology characterizations of MoS2prove that arrayed flakes are homogeneous monolayers, and they are further fabricated as optoelectronic devices showing featured photocurrent loops and stable optical responses. Typical synaptic behaviors of photo‐induced short‐term potentiation, long‐term potentiation, and paired pulse facilitation are recorded under different light stimulations of 450, 532, and 633 nm lasers at various excitation powers. A visual sensing system consisting of 5 × 6 pixels is constructed to simulate the light‐sensing image mapped by forgetting curves in real time. Moreover, the system presents the ability of utilizing associated images to restore vague and incomplete memories, which successfully mimics human intelligent behaviors of association memory and logical reasoning. The work emulates the brain‐like artificial intelligence using arrayed 2D semiconductors, which paves an avenue to achieve smart retina and complex brain‐like system.