According to the present invention, a treatment liquid that includes a solvent and a solute is supplied to a substrate (9). At least one portion of the solvent volatilizes from the treatment liquid, which solidifies or hardens and becomes a particle-holding layer. A removal liquid is supplied to the substrate (9), and the particle-holding layer is removed from the substrate (9). The solute component of the particle-holding layer is insoluble or poorly insoluble in the removal liquid, and the solvent is soluble. When heated to a transformation temperature or higher, the solute component of theparticle-holding layer transforms and becomes soluble in the removal liquid. The removal liquid is supplied after the formation of the particle-holding layer without the solute component having been transformed.