Persistent radicals, species with unpaired electrons, are pivotal for advanced optical and electrical applications but are challenging to stabilize. Herein, we report a melt-quenching vitrification strategy that stabilizes persistent organic radicals within chiral zero-dimensional hybrid zinc chloride glasses, overcoming their intrinsic instability. These radicals are generated via deprotonation-induced organic cations during the vitrification process and are subsequently trapped within the glas