The effects of radiation on a variety of uranyl peroxide compounds were examined using gamma-rays and 5 MeV He ions, the latter to simulate alpha alpha-particles. The studied materials were studtite, [(UO2)(O-2)(H2O)(2)](H2O)(2), the salt of the U-60 uranyl peroxide cage cluster, Li44K16[(UO2)(O-2)(OH)](60)center dot 255H(2)O, the salt of U(60)Ox(30) uranyl peroxide oxalate cage cluster, Li12K48[{(UO2)(O-2)}(60)(C2O4)(30)]center dot nH(2)O, and the salt of the U(24)Pp(12) (Pp = pyrophosphate) uranyl peroxide pyrophosphate cage cluster, Li24Na24[(UO2)(24)(O-2)(24)(P2O7)(12)]center dot 120H(2)O. Irradiated powders were characterized using powder X-ray diffraction, Raman spectroscopy, infrared spectroscopy, X-ray photoelectron spectroscopy, and UV-vis spectroscopy. A weakening of the uranyl bonds of (U60) (w)as found while studtite, U(60)Ox(30), and U(24)Pp(12) were relatively stable to gamma-irradiation. Studtite and U-60 are the most affected by alpha alpha-irradiation forming an amorphous uranyl peroxide as characterized by Raman spectroscopy and powder X-ray diffraction while U(60)Ox(30) and U(24)Pp(12) show minor signs of the formation of an amorphous uranyl peroxide.