Methods of preparing a multi-shell nanocrystal structure, multi-shell nanocrystal structures thus obtained, and a fabricated device including the same are provided. A multi-shell nanocrystal structure may be formed by preparing a core nanocrystal and reacting the core nanocrystal with two or more precursors having different reaction rates to sequentially form two or more layers of shell nanocrystals having different compositions on a surface of the core nanocrystal.