A Quasi‐1D TiS 3 /2H‐MoTe 2 van der Waals Heterostructure for Intelligent Sensing With Decoupled Perception and Memory Functions

The relentless demand for real‐time, high‐dimensional optical information processing is fundamentally hindered by the physical separation of sensing, storage, and computing in conventional architectures, which incurs prohibitive energy and latency overheads. Here, we break this paradigm by constructing a quasi‐one‐dimensional TiS 3 /2H‐MoTe 2 van der Waals heterostructure that intrinsically decouples and synergistically couples two distinct physical mechanisms of anisotropic carrier transport for polarization‐sensitive perception and ion migration/trapping for nonvolatile memory. This TiS 3 /2H‐MoTe 2 heterostructure simultaneously delivers self‐powered, near‐infrared polarization‐senstive photodetection with comparable performance (a dichroic ratio of 7.14, responsivity of 198 mA/W, detectivity of 6.9 × 10 11 Jones, and a fast 61/67 µs response at 1064 nm), alongside robust memristive switching behavior (ON/OFF ratio exceeding 10 5 and retention >2300 s). The versatility is governed by decoupled driving forces of transient photogenerated carrier dynamics and persistent electric‐field‐driven ion and hole migration, enabling physically independent yet co‐located perception and memory channels. Beyond functional synergy, this platform executes a complete bioinspired cognitive chain, from threshold‐triggered nociception and injury‐induced sensitization to real‐time skylight‐polarization navigation, all within a single device. Our work transcends post‐processing compensation and functional additivity, establishing an intrinsic, intelligent paradigm for in‐sensor computing with immediate implications for edge AI, autonomous systems, and neuromorphic electronics.