The development of the information age has made resistive random access memory (RRAM) a critical nanoscale memristor device (MD). However, due to the randomness of the area formed by the conductive filaments (CFs), the RRAM MD still suffers from a problem of insufficient reliability. In this study, the memristor of Ag/ ZrO 2 /WS 2 /Pt structure is proposed for the first time, and a layer of two-dimensional (2D) WS 2 nanosheets was inserted into the MD to form 2D material and oxide double-layer MD (2DOMD) to improve the reliability of single-layer devices. The results indicate that the electrochemical metallization memory cell exhibits a highly stable memristive switching and concentrated ON-and OFF-state voltage distribution, high speed (∼10 ns), and robust endurance (>10 9 cycles). This result is superior to MDs with a single-layer ZrO 2 or WS 2 film because two layers have different ion transport rates, thereby limiting the rupture/rejuvenation of CFs to the bilayer interface region, which can greatly reduce the randomness of CFs in MDs. Moreover, we used the handwritten recognition dataset (i.e., the Modified National Institute of Standards and Technology (MNIST) database) for neuromorphic simulations. Furthermore, biosynaptic functions and plasticity, including spike-timing-dependent plasticity and paired-pulse facilitation, have been successfully achieved. By incorporating 2D materials and oxides into a doublelayer MD, the practical application of RRAM MD can be significantly enhanced to facilitate the development of artificial synapses for brain-enhanced computing systems in the future.