In this Article, we report on a packing scheme of monodisperse colloidal nanospheres by aerosol-assisted clustering. When an aqueous suspension of colloidal nanospheres was sprayed into aerosol droplets by an ultrasonic nebulizer, the nanospheres were encapsulated in the aerosol droplets and the evaporation of water from the droplets at high temperatures led to the packings of nanospheres. The configurations of the colloidal nanospheres minimized the interparticle potential energy or the second moment of mass distribution depending on the number of the constituting nanospheres. Other types of nonspherical microparticles or hollow microclusters were also produced by self-organizing organic-inorganic binary colloids of different sizes in an aerosol spray pyrolysis reactor. The aerosol-assisted fabrication of colloidal clusters was very effective as compared to the method based on oil-in-water or water-in-oil emulsions, in which the removal of residual oil was not easy and time-consuming.