A Smart‐Perception Rare Earth MOF

ABSTRACT Smart responsive luminescent materials have attracted considerable scientific and technological interest owing to their broad optoelectronic applications. However, issues such as single responsive mode, inadequate spectral coverage, and poor environmental adaptability still hinder their diversified development. Herein, we propose the concept of smart multi‐stimuli responsive scintillator (SMRS) and fabricate a new series of rare earth metal–organic frameworks (RE‐MOFs) with active and passive perception capabilities. Such RE‐MOFs exhibit excellent scintillation performances, including high relative light yield (max ∼ 42,200 photons MeV −1 ), low dose rate detection limit (min ∼ 128.2 nGy air s −1 ), and great photostability. Systematic modulation of RE 3+ contents endows MOFs with tunable broadband luminescence, thereby ensuring the passive perception. The distinct photo‐ and radio‐luminescent mechanisms lead to significant spectral contrasts under UV and X‐ray irradiation. Furthermore, RE‐MOFs demonstrate thermal‐stimuli responsive luminescent variation since heat will influence the energy transfer processing among the organic and inorganic units. As a result, RE‐MOFs autonomously produce active luminescent perception toward both irradiation and thermal stimuli. These SMRSs exhibit great potential in in situ optical imaging and high‐security photonic barcodes (the widest spectral range among MOFs for photonic encoding). This study establishes a new paradigm for smart MOF‐based scintillators for an advanced intelligent perception system.