[Object]An object of the present invention is to provide a method for manufacturing an oxide single crystal substrate having less dispersion in characteristics within the substrate surface.[Means to solve the Problems]In the manufacture method of the present invention, a powder containing a Li compound is dispersed in a medium to form a slurry, and heat is applied while the slurry is in contact with the surface of the oxide single crystal substrate, so as to diffuse Li into the substrate from the surface thereof to effect a modification of the substrate; or after the slurry is brought into contact with the surface of the oxide single crystal substrate, the oxide single crystal substrate is buried in a powder containing the Li compound, and heat is applied to effect the diffusion of Li in the substrate from the surface thereof whereby a modification of the substrate occurs.