SnSe/FeSe Memristors for Programmable Multi‐Regime Switching and Neuromorphic Computing

Neuromorphic devices capable of emulating biological synapses have emerged as a promising alternative to conventional computing architectures. Here, solution‐processed 2D SnSe/FeSe nanosheet heterostructures are demonstrated as versatile memristors exhibiting programmable multi‐regime resistive switching. Percolating nanosheet networks with intrinsic defect dynamics enable the coexistence of digital and analog switching. Ag‐electrode devices exhibit digital switching via filamentary electrochemical metallization (ECM), while Ag‐free measurements confirm analog switching driven by vacancy motion and Schottky‐barrier modulation. The ECM‐based devices demonstrate robust endurance (~10 4 cycles), lower switching voltage (< 0.5 V), and high retention as non‐volatile memory elements, while the Ag‐free devices display gradual potentiation and depression, short‐term plasticity and paired‐pulse facilitation, closely mimicking neuronal functions. Moreover, a memristive neural network is simulated using the hardware‐software co‐design and differential pair mapping mechanism, showing performance close to that of a pure software‐based neural network. These findings highlight 2D nanosheet heterostructures as low‐cost, scalable platforms for adaptive, brain‐inspired computing, bridging the gap between memory storage and neuromorphic processing.