Surface oxidation employing neutral oxygen irradiation significantly improves the switching and synaptic performance of ZnO-based transparent memristor devices. The endurance of the as-irradiated device is increased by 100 times, and the operating current can be lowered by 10 times as compared with the as-deposited device. Moreover, the performance-enhanced device has an excellent analog behavior that can exhibit 3 bits per cell nonvolatile multistate characteristics and perform 15 stable epochs of synaptic operations with highly linear weight updates. A simulated artificial neural network comprising 1600 synapses confirms the superiority of the enhanced device in processing a 40 × 40 pixels grayscale image. The irradiation effectively decreases the concentration of oxygen vacancy donor defects and promotes oxygen interstitial acceptor defects on the surface of the ZnO films, which consequently modulate the redox process during rupture and rejuvenation of the filament. This work not only proposes the potential of ZnO-based memristor devices for high-density invisible data storage and in-memory computing application but also offers valuable insight in designing high-performance memristor devices, regardless of the oxide system used, by taking advantage of our neutral oxygen irradiation technique.