In this work, a complex experimental study of the effect of electron and proton ionizing radiation on the properties of carbon nanowalls (CNWs) is carried out using various state-of-the-art materials characterization techniques. CNW layers on quartz substrates were exposed to 5 MeV electron and 1.8 MeV proton irradiation with accumulated fluences of 7 × 10 13 e/cm 2 and 10 12 p/cm 2, respectively. It is found that depending on the type of irradiation (electron or proton), the morphology and structural properties of CNWs change; in particular, the wall density decreases, and the sp 2 hybridization component increases. The morphological and structural changes in turn lead to changes in the electronic, optical, and electrical characteristics of the material, in particular, change in the work function, improvement in optical transmission, an increase in the surface resistance, and a decrease in the specific conductivity of the CNW films. Lastly, this study highlights the potential of CNWs as nanostructured functional materials for novel high-performance radiation-resistant electronic and optoelectronic devices.