The titanium nitride–aluminum oxide–silicon nitride–silicon oxide–silicon devices with a high-k aluminum oxide as a charge-blocking layer (TANOS) could be candidates for nonvolatile total ionization dose (TID) radiation sensors. Gamma radiation induces a significant decrease in the threshold voltage VT of TANOS and the radiation-induced VT decrease of TANOS is nearly 1.5 times that on a standard titanium nitride–silicon oxide–silicon nitride–silicon oxide–silicon (TONOS) device after 10 Mrad TID gamma irradiation. The change in VT of TANOS after gamma irradiation also has a strong correlation to the TID up to 10 Mrad gamma irradiation. The VT retention characteristics of TANOS devices can be improved before gamma irradiation and after 10 Mrad gamma irradiation. Moreover, the VT retention characteristics of TANOS devices can be markedly improved and are nearly 10% better than those of standard TONOS devices after 10 Mrad gamma irradiation. Therefore, the TANOS device in this study has demonstrated the possibility of its use for high response and good TID data retention for nonvolatile TID radiation sensing.