Tao Hu, Yulan Guo, Xiaodong Yi, Ming Zhao, Yan Gao, Hang Lin
ABSTRACT Smart multi‐stimuli‐responsive luminescence materials, which integrate diverse optical functionalities and hold significant promise for cutting‐edge optoelectronic applications, have advanced notably in recent years. However, traditional phosphor powders often suffer from instability due to organic binders, limiting their practical utility. This study presents a novel multi‐responsive luminescent glass ceramic (GC) based on SrMg 2 Al 6 Si 9 O 30 :Eu 2+ osumilite, developed via an in situ glass crystallization strategy. The material uniquely integrates efficient and stable photoluminescence (PL, quantum yield 76%), persistent luminescence (PersL), thermally stimulated luminescence (TSL), and X‐ray‐excited radioluminescence (RL, light yield 13 856 photons/MeV) in a single, intrinsically stable matrix. Molecular dynamics simulations reveal that the precursor glass exhibits crystal‐like topological configurations, promoting nucleation of the SrMg 2 Al 6 Si 9 O 30 :Eu 2+ phase with a low crystallization activation energy (226.7 kJ/mol). The GC demonstrates exceptional thermal stability and robust performance in applications: high‐security anti‐counterfeiting via dynamic multi‐mode (PL/PersL/TSL) information encoding, and X‐ray detection with 8 lp/mm spatial resolution, outperforming commercial scintillators like BGO. These findings establish a new paradigm for designing stable, multi‐responsive luminescent materials, paving the way for next‐generation integrated optical devices.