A method for preparing a multilayer of nanocrystals. The method includes the steps of (i) coating nanocrystals surface-coordinated by a photosensitive compound, or a mixed solution of a photosensitive compound and nanocrystals surface-coordinated by a material miscible with the photosensitive compound, on a substrate, drying the coated substrate, and exposing the dried substrate to UV light to form a first monolayer of nanocrystals, and (ii) repeating the procedure of step (i) to form one or more monolayers of nanocrystals on the first monolayer of nanocrystals. Further, an organic-inorganic hybrid electroluminescence device using a multilayer of nanocrystals prepared by the method as a luminescent layer. The luminescent efficiency and luminescence intensity of the electroluminescence device can be enhanced, and the electrical properties of the electroluminescence device can be controlled by the use of the multilayer of nanocrystals as a luminescent layer.