An efficient method for preparing a highly-directional highly-dense two-dimensional material film. The method comprises: using a circular tube with a smooth inner surface as a casting mold; and pouring a solution containing a two-dimensional material into the mold when the mold rotates at high speed in a circumferential direction, wherein the solution is uniformly coated on the inner surface of the mold by centrifugal force, the centrifugal rotation generating a shearing force that causes the two-dimensional material to be directionally and regularly arranged layer upon layer in a circumferential direction in the solution, and, the centrifugal force facilitates highly-dense accumulation of the two-dimensional material, thereby obtaining a highly-directional highly-dense two-dimensional material film. The method is applicable in the preparation of a variety of two-dimensional materials such as graphene, a composite material film thereof, and a laminated heterostructure film, and greatly improves electrical, thermal, and mechanical properties of a film.