In article number 1806646, Gunuk Wang and co-workers, inspired by light-assisted dopamine-facilitated synaptic activity, which achieves rapid learning and adaptation by lowering the threshold of the synaptic plasticity, fabricate and design a two-terminal organolead halide perovskite-based photonic synapse in which the synaptic plasticity is modified by both electrical pulses and light illumination. Such controllability enables high-order tuning of synaptic plasticity.