A composite structure formation method includes the steps of storing a plurality of pre-formed controlled particles in a storage mechanism, supplying the controlled particles from the storage mechanism to an aerosolation mechanism constantly, disaggregating the supplied controlled particles into a plurality of the fine particles in the aerosolation mechanism to form an aerosol in which an entire contents of the controlled particles including the fine particles are dispersed in the gas; and spraying all of the fine particles in the aerosol toward the substrate to form a composite structure of the structure and the substrate. The controlled particles are controlled so that bonding strength between the fine particles includes a mean compressive fracture strength sufficient to substantially avoid disaggregation during the supply step, but which permits the controlled particles to be substantially completely disaggregated in the disaggregation step.