<p>Glass scintillators are promising for large-scale radiation detection but traditionally suffer from low light yield and slow response. Here, we present highly transparent, homogeneous, and size-customizable organic-inorganic hybrid scintillating glasses, combining an inorganic glass host with organic components. The resulting hybrid glasses exhibit excellent radiation response, including rapid luminescence decay and enhanced scintillating efficiency. Notably, they achieve superior α-particle detection performance. In addition, their low density enables selective α-particle detection in mixed radiation fields and minimizes γ-ray interference, outperforming conventional glass scintillators. Furthermore, the glasses can be doped with elements such as lithium, boron, and gadolinium, offering efficient thermal neutron detection. These findings highlight the potential of organic-inorganic hybrid glasses as advanced scintillating materials for high-energy radiation field detection, with enhanced functionality for applications in nuclear medicine, oil exploration, and nuclear safety.</p>