The nonvolatile memory characteristics of metal–oxide–semiconductor (MOS) structures containing Au nanocrystals in the Al2O3/SiO2 matrix were studied. In this work, we have demonstrated that the use of Al2O3 as control oxide prepared by atomic-layer-deposition enhances the erase speed of the MOS capacitors. A giant capacitance–voltage hysteresis loop and a very short erase time which is lower than 1 ms can be obtained. Compared with the conventional floating-gate electrically erasable programmable read-only memories, the erase speed was promoted drastically. In addition, very low leakage current and large turn-around voltage resulting from electrons or holes stored in the Au nanocrystals were found in the current–voltage relation of the MOS capacitors.