Flexible memristor is one of the most promising wearable devices for abundant data storage and processing. In this work, interface engineering by inserting the Al 2 O 3 barrier layer is carried out to construct Pt/TiO x /Al 2 O 3 /Pt/indium tin oxide (ITO) flexible artificial synapse device. The memristor performance can be maintained even under 1000 times of bending without degradation, demonstrating its excellent mechanical property. With the Al 2 O 3 diffusion barrier layer, the oxygen vacancies ( ${V}_{\text {o}}$ ) movement is slowed down for filaments formation and rupture, thus it boosts up the synaptic plasticity, including long-term potentiation/depression, paired-pulse facilitation (PPF), and spike-timing-dependent plasticity (STDP). Moreover, on the basis of the enhanced symmetry and linearity of conductance for Pt/TiO x /Al 2 O 3 /Pt/indium tin oxide (ITO) memristor, the neural network simulation for supervised learning presents an online learning pattern recognition, the accuracy can achieve to 91.15%. Overall, the Pt/TiO x /Al 2 O 3 /Pt/ITO memristor with excellent flexibility is a promising emulator for biological synapses, which could be beneficial to future flexible memristor-based neuromorphic computing.