Bimodal Mechanoluminescent Core‐Sheath Yarns With Multi‑Stage Excitation for Self‑Powered, Long‑Afterglow Wireless Intelligent Textiles

ABSTRACT Inspired by marine organisms (e.g., anglerfish and aquatic firefly larvae) that synchronize environmental perception with luminescence, optoelectronic bimodal sensors have garnered considerable attention for their immense potential in extreme scenarios such as underwater rescue. However, the efficient integration and precise regulation of heterogeneous stimulus response capabilities still remain challenging, especially in intelligent textiles, which play a significantly important role in future human–machine interfaces. Herein, a yarn‐scale multilayered structure strategy for multifunctional integration was proposed, and a self‐powered yarn with both mechanoluminescence (ML) and afterglow emission was successfully fabricated. Integrating SrAl 2 O 4 :Eu 2+ , Dy 3+ (SAOED) as a secondary luminescent component, the synergy of triboelectric charge transfer and enhanced friction yields a 203.4% ML enhancement and enables a re‐excited long‐lasting afterglow. Via the embroidery process, the yarn was integrated into intelligent textiles with controllable paths and patterns, thereby achieving the customized integration and on‐demand distribution of self‐powered and visualized sensing functions. Moreover, a system based on machine learning analysis and Bluetooth transmission was also developed, enabling precise motion recognition (accuracy> 92%) and intelligent control for underwater rescue operations, while providing bimodal wireless and visual alerts. This work establishes a novel paradigm for the practical implementation of next‐generation interactive textiles in deep‐sea environments.