This study used the powder metallurgy method to create aluminum oxynitride (AlON)-reinforced zircoborate glass-ceramic composites. The solid-phase reaction method was used to synthesize AlON powder, which was then added to Zr-based glass-ceramic in different amounts (0, 4, and 8 % by weight) to make it stronger and harder. The prepared materials were characterized for their structural, physical, and radiation shielding properties. The density of GZr8 (AlON-free) had a value of 2.9 g/cm3, and the sintered glass-ceramic density with 4 % wt. AlON reinforcement (GZr8Al4) reached 3.05 g/cm3. The highest density of 3.11 g/cm3 was obtained for the GZr8Al8 sample with 8 % AlON wt. The Vickers hardness for GZr8, GZr8Al4, and GZr8Al8 was measured to be 4.89, 5.94, and 6.33 GPa, respectively. The AlON-reinforced GZr8 samples had fast neutron (FN) removal cross-sections of 0.0796 cm−1 and 0.0824 cm−1 for AlON content of 4 and 8 wt%, respectively. Generally, the coherent scattering cross-section (σcoh), incoherent scattering cross-section (σinc), and absorption cross-section (σabs) of thermal neutrons (TNs) increase from 0.047856 cm−1, 0.02072 cm−1, and 0.01498 cm−1, respectively for GZr8 to 0.53124 cm−1, 0.02074 cm−1, and 0.01795 cm−1, for GZr8Al8. AlON was proven to improve the ability of the Zr-based glass-ceramics to attenuate FNs and TNs. Stopping powers of electrons, protons, alpha particles and carbon ions increase with the AlON content of the materials. Comparatively, the range of charged radiation in AlON-rich samples is lower. The inclusion of AlON in the matrix of the Zr-based glass-ceramics makes it more efficient at absorbing charged radiation and can be used in ion beam or hadron therapy, ion beam analysis, or other charged radiation environments as an absorber.