Memristors can be used to mimic synaptic behavior in artificial neural networks, which makes them a key component in neuromorphic computing and holds promise for advancing the field. In this study, a memory artificial synaptic device based on ZnO−BaTiO 3 (ZnO−BTO) vertically aligned nanocomposite thin films was prepared. The vertical interface between the two phases can be used as a conduit for oxygen vacancy (OV) accumulation and a channel for OV movement, which greatly optimizes the resistive switching performance of the device and has the potential for multistage storage. By applying different pulse sequences to the device, the conductance of the device is adjusted from multiple angles, and a variety of synaptic functions are simulated, such as paired-pulse facilitation, spiketiming-dependent plasticity, short-term plasticity to long-term plasticity (STP−LTP), and long-term potentiation/depression (LTP/LTD). Finally, we construct a neural network for image recognition, and the recognition accuracy can reach 91%. Our study demonstrates the feasibility of using composite thin-film vertical interface to regulate the resistive performance of memristors and its great potential in artificial synaptic simulation and neuromorphic computing.