A method for producing a crystal film of an organic compound from a molten liquid or solution of the organic compound on a substrate or between a pair of substrates, the substrate or at least one of the pair of substrates having on a part of the surface thereof a three-dimensional geometrical structure capable of controlling the direction of the crystal growth of the organic compound, and the other part of the surface thereof than the part having a three-dimensional geometrical structure being smooth. The resulting crystal film comprises a sufficiently large single crystal for application to a practical element with its orientation controlled in an arbitrarily selected direction.