In particular, the fluorescence inks could be easily printed on the banknote, ID card, passport, and packaging of the product; accordingly, the anti-counterfeiting technology based on fluorescence tags has been highlighted with low cost, high-security level, and facile decryption process that can be directly recognized by the ultraviolet (UV) lamp. [35] For instance, the emission of A 2 AgX 3 (A = Rb, Cs; X = Cl, Br, I) could be facilely regulated by changing the composition, showing the application potential in fluorescence anti-counterfeiting. [36] Nevertheless, the limited response range makes traditional UV light-activated anti-counterfeiting fluorescence tags unsatisfactory for the requirements of high-level anticounterfeiting applications. Therefore, exploring complicated anti-counterfeiting fluorescent materials whose response range can be broadened from UV to near-infrared (NIR) light and even X-rays are urgently needed. The fluorescent materials with a down-conversion response require a suitable energy gap that the UV light could activate. However, the traditional metal-oxide semiconductors possess a wide bandgap; thus, it is necessary to introduce lanthanide metal ions to act as activators. [37] The up-conversion photoluminescence (UCPL) process usually involves photosensitizers (Yb 3+ , etc.) to absorb infrared light and transfer the absorbed energy to other luminescent species. [38] Nonetheless, the multi-photon absorption process usually occurs under the irradiation of high-power laser (e.g., >1 kW cm −2 ), hampering the application in practical scenarios. Moreover, the doping amount of photosensitizers is critical for the final emissive behaviors and lacks batch-to-batch and labto-lab reproducibility. In terms of X-ray scintillators, except for extraordinary luminescence efficiency, the attenuation capability to X-ray becomes another critical criterion for screening the efficient scintillators, which requires the participation of heavy atoms, such as metal and iodine elements. Overall, it is still challenging to synthesize a single-source material with response to UV, NIR, and X-ray simultaneously.Recently, the outstanding photophysical performance of metal halide perovskites and derivatives has brought them to the research forefront of luminescent materials. For instance, the 3D CsPbX 3 (X = Cl, Br, and I) nanocrystals show extraordinary down-conversion properties due to the spatial confinement of excitons within nanocrystals. [39][40][41] Fortunately, lowering down the crystal structure dimensionality is another strategy Anti-counterfeiting has become a serious issue around the global world; fluorescence-based tags are praised for the low-cost and facile decryption process. However, the high-level anti-counterfeiting application requires incorporating multifunctional luminescent materials with response to different excitation sources. Herein, a dimeric Cu(I)-halide-clusters-assembled singlecrystal (AEP) 2 Cu 2 I 6 •2I•2H 2 O (AEP = N-aminoethylpiperazinium) concerning a high down-conversion photol...