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.