The present method of manufacturing a GaN-based film includes the steps of preparing a composite substrate, the composite substrate including a support substrate in which a coefficient of thermal expansion in a main surface is more than 0.8 time and less than 1.2 times as high as a coefficient of thermal expansion of GaN crystal in a direction of a axis and a single crystal film arranged on a side of the main surface of the support substrate, the single crystal film having threefold symmetry with respect to an axis perpendicular to a main surface of the single crystal film, and forming a GaN-based film on the main surface of the single crystal film in the composite substrate. Thus, a method of manufacturing a GaN-based film capable of manufacturing a GaN-based film having a large main surface area and less warpage is provided.