luminescence. With the booming of materials discovery, considerable progress has been witnessed in the development of luminescent materials, accompanied by diverse optical properties. [4] Multimodal luminescence with multi-level performance by increasing the luminescence modes has attracted extensive interest in recent years. [5] Multimodal luminescence generally involves tunable photon emissions in response to various external stimuli, which could represent good confidentiality abilities for anti-counterfeiting or encryption technologies. For instance, Xia and coworkers realized distinct long persistent luminescence, short-lived UCL in NaGdTi 2 O 6 :Pr 3+ , Er 3+ phosphor which responded to a wide spectrum ranging from X-ray to sunlight, thermal disturbance, and mechanical force. [6] Great efforts have been made to achieve the integration of multiple optical characteristics for sophisticated applications with the combination of UCL, DS, thermally/optically/ mechanically/Xray stimulated luminescence, persistent luminescence, and/or photochromism. [7] Inorganic phosphors, one of the most important types of luminescent materials, have been widely employed in fabricating optoelectronic devices. To obtain multimode-responsive inorganic phosphor-based materials, triple or even quadruple doping ions (e.g., lanthanides, main group, and transition metal ions) or a series of hosts with different compositions were frequently used. Specifically, lanthanide ions including Yb 3+ , Er 3+ , Sm 3+ , Ho 3+ , Nd 3+ , and Tm 3+ have been widely recognized for the exceptional luminescence due to their unique 4f electronic configurations and abundant energy levels. For instance, Yan et al. successfully synthesized the Yb 3+ /Er 3+ /Bi 3+ tri-doping double perovskite with the multimodal luminescent performance. [8] Pan and coworkers first designed up-converted persistent luminescence from Zn 3 Ga 2 GeO 8 :Cr 3+ ,Yb 3+ ,Er 3+ phosphors by combining UCL and long-persistent luminescence processes. [9] Recently, Lyu et al. developed a smart perovskite LiTaO 3 :Bi 3+ ,Tb 3+ ,Ga 3+ ,Ge 4+ with high charge carrier storage capacity for stress sensing and X-ray imaging applications. [10] Moreover, Sun et al. designed lanthanide doped dumbbell-like core-shell-shell nanocrystal NaErF 4 :Ce 3+ ,Yb 3+ @NaYF 4 :Yb 3+ @ NaNdF 4 :Yb 3+ with UCL/DS switchable emission modes of visible and NIR-II toward deep learning fluorescence bioimaging and in vivo information security. [11] Obviously, to achieve the multi-mode luminescence performance, the combination of multi-ion doping or a series of luminescent materials was Multimode-responsive luminescence materials play pivotal roles both in understanding the fundamental photophysical processes and fabricating smart devices. To obtain inorganic phosphor-based multi-responsive materials, however, triple or even quadruple doping ions or a series of hosts with different compositions are frequently used. In this work, a single-rareearth-doped phosphor, Sr 2 YGaO 5 :Sm 3+ , with multi-responsive luminescence i...