Zero-dimensional (0D) scintillation materials have drawn tremendous attention due to their inherent advantages in the fabrication of flexible high-energy radiation scintillation screens by solution processes. Although considerable progress has been made in the development of 0D scintillators, such as the current leading lead-halide perovskite nanocrystals and quantum dots, challenges still persist, including potential issues with self-absorption, air stability, and eco-friendliness. Here, we present a strategy to overcome those limitations by synthesis and self-assembly of a new class of scintillators based on metal nanoclusters. We demonstrate the gram-scale synthesis of an atomically precise nanocluster with a Cu-Au alloy core exhibiting high phosphorescence quantum yield, aggregation-induced emission enhancement (AIEE) behavior, and intense radioluminescence. By controlling solvent interactions, the AIEE-active nanoclusters were self-assembled into submicron spherical superparticles in solution, which we exploited as a novel building block for flexible particle-deposited scintillation films with high-resolution X-ray imaging performance. This work reveals metal nanoclusters and their self-assembled superstructures as a promising class of scintillators for practical applications in high-energy radiation detection and imaging.