A method of manufacturing a structure in which a substrate can be removed easily from a structure that has been formed on the substrate by using a film forming technology. The method of manufacturing a structure includes the steps of (a) forming an intermediate layer on a substrate; (b) forming a structure including a brittle material layer on the intermediate layer by at least using a spray deposition method of spraying material powder toward the substrate, on which the intermediate layer is formed, to deposit the material powder; and (c) removing the substrate from the structure.