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The synapse is one of the fundamental elements in human brain performing functions such as learning, memorizing, and visual processing. The implementation of synaptic devices to realize neuromorphic computing and sensing tasks is a key step to artificial intelligence, which, however, has been bottlenecked by the complex circuitry and device integration. We report a high-performance charge-trapping memory synaptic device based on two-dimensional (2D) MoS2 and high-k Ta2O5–TiO2 (TTO) composite to build efficient and reliable neuromorphic system, which can be modulated by both electrical and optical stimuli. Significant and essential synaptic behaviors including short-term plasticity, long-term potentiation, and long-term depression have been emulated. Such excellent synaptic behaviors originated from the good nonvolatile memory performance due to the high density of defect states in the engineered TTO composite. The 2D synaptic device also exhibits effective switching by incident light tuning, which further enables pattern recognition with accuracy rate reaching 100%. Such experimental demonstration paves a robust way toward a multitask neuromorphic system and opens up potential applications in future artificial intelligence and sensing technology.