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Herein, the first study on the scintillation properties of CsCu2X3 and Cs3Cu2X5 (where X: Cl−, Br−, I−) is presented, describing their charged particle‐induced luminescence involving electrons, protons, α‐particles, and heavy ions, as well as revealing their capabilities on the timing and spectroscopic evaluation of single‐particle events. The thin layers are prepared with a simple and cost‐effective deposition procedure, without the incorporation of external dopants, exploiting the intrinsic radiative recombination observed in low‐dimensional perovskites. The combined effect of the high binding energy and localized stability of self‐trapped excitons, large Stokes shift, defect tolerance, and the high excitation density along the particle track leads to the emergence of boosted scintillation pulses. The observations demonstrate the first use of inorganic thin‐film scintillators with optical pulse characteristics and light yield competitive with doped single crystal scintillators, while also providing improved structural and functional stability under extreme environmental conditions. [ABSTRACT FROM AUTHOR]