Ziyi Fang, Xiaofeng Pan, Qi’an Zhang, Mingzhi Wu, Yang Liu, Qidong Ma, Biyun Ren, Yue Wang, Shengqiang Liu, Maryam Zulfiqar, Ming‐Gang Ju, Jiulin Gan, Leipeng Li, Feng Wang, Dengfeng Peng
Abstract Materials exhibiting mechanoluminescence (ML) that directly convert mechanical stimuli into light hold significant potential for real-time stress sensing and intelligent photonic systems. However, most high-performance ML systems rely on complex multicomponent compounds that often suffer from limited intensity, stability, and scalability, largely due to poorly understood mechanisms. Herein, we report a simple Al 2 O 3 :Cr 3+ oxide that exhibits unprecedented ML intensity, enabled by a well-defined mechanical-to-optical energy conversion process. The self-recoverable ML arises from stress-induced ionization of electrons from luminescence centers, followed by their recapture upon stress release. By precisely tuning the doping levels, annealing conditions, and heterojunction interfaces, Al 2 O 3 :Cr 3+ phosphors achieved intense, reproducible, and thermally stable near-infrared emission. Notably, high-temperature annealing dramatically enhanced the ML intensity, with thermodynamic and kinetic analyses revealing increases in the carrier and defect concentrations by several orders of magnitude, accounting for the exceptional brightness. By leveraging the chemical robustness, abundance, and low cost of alumina, we demonstrated the flexible ML paper for stress visualization and multi-level anti-counterfeiting, as well as in-situ grown Al 2 O 3 :Cr 3+ luminescent layers on Cr–Al alloys for passive, real-time stress monitoring. This study establishes Al 2 O 3 as a durable and scalable oxide platform for next-generation self-recoverable ML materials, bridging fundamental research and practical sensing technologies.