The self-organization of CdSe nanocrystallites into three-dimensional semiconductor quantum dot superlattices (colloidal crystals) is demonstrated. The size and spacing of the dots within the superlattice are controlled with near atomic precision. This control is a result of synthetic advances that provide CdSe nanocrystallites that are monodisperse within the limit of atomic roughness. The methodology is not limited to semiconductor quantum dots but provides general procedures for the preparation and characterization of ordered structures of nanocrystallites from a variety of materials.