This study characterizes the charge storage characteristics of metal/HfO2/Au nanocrystals (NCs)/SiO2/Si and significantly improves memory performance and retention time by annealing the HfO2 blocking layer in O2 ambient at 400°C. Experimental evidence shows that the underlying mechanism can be effectively applied to reduce oxygen vacancy and suppress unwanted electron trap-assisted tunneling. A memory window of 1 V at an applied sweeping voltage of ±2 V is also shown. The low program/erase voltage (±2 V) and the promising retention performances indicate the potential application of NCs in low-voltage, non-volatile memory devices.