Surface potential decay on negative corona charged epoxy/Al2O3 nanocomposites irradiated with high-energy electron beam has been investigated in this paper. 2-mm-thick laminate nanocomposite samples were irradiated with electron beam at an average energy of 7.5 MeV, and the total accumulated dose was up to 500 kGy. After the irradiation, the nanocomposites were corona charged with dc voltage at −10 kV through a pair of needle to plate electrode. Surface potential of the sample was then measured by means of an electrostatic voltmeter through which trap distribution and carrier mobility were calculated. Differential scanning calorimetry curve for the each sample was measured to understand the change in chemical and physical structures induced by the irradiation. Results obtained indicated that the presence of nanofiller in the nanocomposites played a role in limiting the charge transportation both before and after the irradiation, and the charge transportation behavior was remarkably dependent upon the total irradiation dose. It is found that when irradiated with a certain total dose of electron beam, electron migration within epoxy and its nanocomposites is restricted, which should be attributed to the high-energy irradiation-induced structural change of the material.