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The human visual system to process real‐time light signals and safeguard against excessive light exposure serves as a model for artificial vision systems. Despite the wide use of optoelectronic synaptic devices in such simulations, their complex circuitry and high energy consumption have impeded further development. Herein, a biomimetic ocular system utilizing organic all‐photonic synapses is constructed to realize sensation, memory, processing, and protective light reflex abilities. The synaptic performances are facially regulated by simple molecular engineering to afford a record PPF value of 430%. Impressively, a large area (400 cm2) synaptic device with a high uniformity (96%) exhibited four fundamental functions of an ocular system for the first time, which significantly simplified the circuit system and reduced energy consumption. This work provides a facial strategy to construct all‐photonic synapses, holding great potential in prosthetics and neurorobotics. [ABSTRACT FROM AUTHOR]