AbstractExploitation of the oxidation behaviour in an environmentally sensitive semiconductor is significant to modulate its electronic properties and develop unique applications. Here, we demonstrate a native oxidation-inspired InSe field-effect transistor as an artificial synapse in device level that benefits from the boosted charge trapping under ambient conditions. A thin InO_x layer is confirmed under the InSe channel, which can serve as an effective charge trapping layer for information storage. The dynamic characteristic measurement is further performed to reveal the corresponding uniform charge trapping and releasing process, which coincides with its surface-effect-governed carrier fluctuations. As a result, the oxide-decorated InSe device exhibits nonvolatile memory characteristics with flexible programming/erasing operations. Furthermore, an InSe-based artificial synapse is implemented to emulate the essential synaptic functions. The pattern recognition capability of the designed artificial neural network is believed to provide an excellent paradigm for ultra-sensitive van der Waals materials to develop electric-modulated neuromorphic computation architectures.