This paper reports an enhancement of the nonvolatile memory characteristics of GaN/AlN resonant tunnelling diodes (RTDs) by reducing the crystal defects in the quantum well structure. Pit-shaped crystal defects are strongly suppressed when pure N2, instead of a N2/H2 mixture, is used as a carrier gas and trimethylindium is introduced as a surfactant for metalorganic vapor phase epitaxy of the quantum well structure. In addition, the density of dislocations is lowered by controlling the growth conditions and structure of the buffer layer between a GaN/AlN RTD and a sapphire (0001) substrate. The leakage current through the quantum well structure is lowered, and an extremely high ON/OFF of >1300, which is 20 times higher than the values obtained in previous studies, is induced. Theoretical calculations based on Poisson’s equation and the Tsu–Esaki formula indicate that a high ON/OFF ratio of >103 can be enhanced by increasing the density of electrons accumulating in the quantum well to a level on the order of 1018 cm–3. Furthermore, nonvolatile memory operations were performed by inputting the sequential pulse voltages with a speed of with nanosecond time scale which is faster than speeds of electron release from the crystal defects. These results strongly indicate that the nonvolatile memory characteristics of GaN/AlN RTDs are due to intersubband transitions and electron accumulation in the quantum well and are not attributed to electron trapping by the crystal defects.