AbstractIt is crucial to develop advanced optoelectronic devices that incorporate multiple functions, including sensing, storage, and computing, which is considered at the forefront of semiconductor optoelectronics to meet emerging functional diversification. In this study, by stacking the n‐type Ga2O3 with the n‐type MoS2 flakes, a Ga2O3/MoS2 heterostructure optoelectronic device with high rectification ratio of ≈105 and on/off ratio of ≈108 is fabricated, which achieves high detectivity of 1.34 × 109 Jones and high responsivity of 28.92 mA/W. More importantly, the Ga2O3/MoS2 heterostructure device shows potential ability to integrate sensing and memorizing, simultaneously, which can be used as artificial neuromorphic synaptic. The device exhibits excellent photo‐induced synaptic functions including short‐term plasticity, long‐term plasticity, and paired‐pulse facilitation, realizing the ability to couple light and electrical signals by Pavlovian associative learning. At last, the device also demonstrates the information processing ability to act as optoelectronic logic gate AND by synergistically regulating the light on/off states and gate voltage. The research introduces an innovative strategy for the development of next‐generation optoelectronic devices which are highly integrated with sensing, memory, and logic processing functions, demonstrating great application prospects in constructing an efficient artificial neuromorphic visual and logic systems.