Yuefei Xiang, Lei Zhong, Minghao Wang, Maofeng Hua, Xiong Pan, Hao Suo, Lei Zhou, Mingmei Wu
ABSTRACT Integrating the dual capabilities of X‐ray detection/imaging and radiation thermometry into a single scintillator through rational materials design opens a new avenue toward advanced multi‐functional radiation‐sensing applications. However, developing the functional material remains a challenge. Here, we report a multifunctional X‐ray induced persistent luminescence (PersL) SrZnP 2 O 7 (SZPO):Dy,Tb phosphor for multimodal sensing applications, including stress monitoring, X‐ray detection/imaging, and radiation thermometry. Upon ultraviolet (UV) light and X‐ray excitation, an efficient energy transfer (ET) from Dy 3+ to Tb 3+ occurs via an electric dipole–dipole interaction mechanism. The phosphor also exhibits pronounced mechanoluminescence (ML), that enables real‐time structural health monitoring and visual stress distribution mapping in building structures such as bridges. Furthermore, flexible films fabricated with SZPO:Dy,Tb demonstrate excellent recoverable PersL and radioluminescence (RL) with retained anti‐thermal quenching (ATQ) behavior, facilitating delayed X‐ray imaging and reliable high‐temperature detection. By exploiting the distinct temperature‐dependent RL responses of the Dy 3+ and Tb 3+ emissions, we achieve high‐performance radiation‐excited optical thermometry with superior sensing performance. This work not only presents an integrated phosphor platform for multi‐scenario radiation sensing but also provides a viable design paradigm for developing advanced functional materials in X‐ray technology and thermometric applications.