AbstractOwing to their unique chemical reactivities and paramagnetism, organic radicals with unpaired electrons have found widespread exploration in physical, chemical, and biological fields. However, most radicals are too short‐lived to be separated and only a few of them can maintain stable radical forms via stereochemical strategies. How to utilize these raw radicals for developing stable radical‐containing materials have long been a research hotspot for many years. This perspective introduces fundamental characteristics of organic radical materials and highlights their applications in biomedical fields, particularly for bioimaging, biosensing, and photo‐triggered therapies. Molecular design of these radical materials is considered with reference to their outstanding imaging and therapeutic performances. Various challenges currently limiting the wide applications of these organic radical materials and their future development are also discussed.