High‐Performance Te Nanowires/MoS₂/Polyimine Nanocomposite‐Based Self‐Healable, Recyclable and Screen‐Printable Flexible Photodetector for Image Sensing

Abstract Intrinsically flexible photodetectors are compelling building blocks for next‐generation wearable optoelectronic systems owing to their distinctive advantages of reliable structural durability and versatile scalability for large‐scale production. However, their practical applications are still impeded by the inferior photodetection performance, irreversible device failure after breakage, and serious e‐waste accumulation after service life. Herein, a high‐performance intrinsically flexible, mechanically durable, self‐healable, closed‐loop recyclable, and screen‐printable Te NWs/MoS₂ nanosheets/polyimine nanocomposite‐based photodetector are designed by engineering‐ordered‐bridged 1D/2D carrier percolation “fast lanes” in dynamic covalent polyimine matrix via a flow‐designed solution‐shearing method. Such a design provides a sixfold, 20.1‐fold, and 6.9‐fold enhancement in carrier mobility, responsivity (11.68 mA W⁻¹), and detectivity (1.145 × 10¹⁰ Jones), respectively, as well as stable photoresponse over eight months or after 50 000 bending‐flattening times. Meanwhile, this photodetector presents excellent self‐healing efficiency and repeatable recyclability for device reconfiguration. Furthermore, these merits can be fully integrated onto textile by assembling nacre‐like Te NWs/MoS₂/polyimine nanocomposite coatings on textiles via screen‐printing processes, enabling programmable patterning of photodetection arrays for large‐area image sensing. This work provides a viable approach for the design of shape‐tunable optoelectronics with reliable mechanical durability and customizable functionalities, demonstrating the tremendous potential for large‐scale applications in wearable optoelectronic systems.