The invention discloses a preparation method of a graphene oxide nano roll and a composite material thereof, which belong to the field of preparation of carbon nano materials. According to the invention, the defects of complex process, low efficiency, high energy consumption, complex process, single product and the like of the existing preparation method of the carbon nano roll and the composite material are overcome. The method comprises the following steps: ultrasonically dispersing graphene oxide sponge prepared by adopting a liquid phase stripping method and freeze-drying in deionized water; dissolving graphene oxide in water, dropwise adding to a clean substrate, horizontally placing in equipment connected with a vacuum pump, and vacuumizing at normal temperature to quickly evaporatewater, thereby obtaining the graphene oxide nano roll; and obtaining a one-dimensional or three-dimensional network structure by controlling the concentration of the graphene oxide; preparing the GO-carbon tube nanoscroll or the GO-carbon tube-metal salt nanoscroll composite material by selectively adding acidified carbon nanotubes and various metal salts. The method is low in cost, easy to operate, high in safety and convenient for large-scale preparation, popularization and application of various products.