We propose a method to fabricate a Ni nanocrystal structure by simultaneously coevaporating Ni and SiO2 pellets. An 800°C rapid thermal annealing was used to enhance the Ni nanocrystals to aggregate. Transmission electron microscopy indicates that the formed Ni nanocrystals show a high density distribution of about 4.5×1012 cm-2. Then, the memory device using the Ni nanocrystals as charge-trapping centers was fabricated. The Ni nanocrystal memory device has an obvious memory window under capacitance–voltage measurement. X-ray photoelectron spectroscopy confirms the memory effect results from the Ni nanocrystals embedded in the SiO2 dielectric layer. Moreover, related reliability characteristics have been extracted.