Interfacial Engineering of Cs 3 Bi 2 Br 9 /MoS 2 Heterostructure‐based Memristors for Self‐rectifying and Nociceptor Applications

ABSTRACT Halide perovskite‐based memristors have demonstrated great potential in neuromorphic computing, yet their performance remains severely limited by poor stability arising from its abundant grain boundaries and intrinsic defects. In this work, we report lead‐free Cs 3 Bi 2 Br 9 perovskite‐based memristors enabled by interfacial engineering with molybdenum disulfide (MoS 2 ). Acting as a growth template, MoS 2 effectively induces the formation of perovskite films with enhanced crystallinity, superior interface quality, and suppressed defects. The constructed Au/Ag/Cs 3 Bi 2 Br 9 /MoS 2 /ITO memristive device achieves typical self‐rectifying behavior with an ultra‐low set voltage of ∼0.14 V, low set power consumption of 140 nW, and low energy of 300 pJ. Meanwhile, the device demonstrates exceptional cycling stability and low device‐to‐device variability (C V < 6.37%). The experimental and theoretical fittings reveal that the resistive switching mechanism is governed by an Ag + ‐assisted trap‐controlled electronic transport, while the reinforced built‐in electric field endows the device with pronounced self‐rectifying characteristics, thereby effectively suppressing sneak currents in crossbar arrays. The device successfully emulates key nociceptive behaviours of biological pain receptors, including threshold response, adaptation, and hyperalgesia. This study highlights the interfacial engineering enables synergistic optimization of crystallinity and defect states. These findings provide new insights into the design of lead‐free perovskite‐based memristors for bioinspired neuromorphic sensory systems.