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Graphene and its derivatives are widely used in various fields due to their unique two-dimensional lamellar structure. This study aims to synthesize ultra-large graphene oxide (GO) sheets from natural flake graphite and investigate the factors influencing their size. Using a two-intercalation method based on the modified Hummers' method, we address the challenge of intercalating large-diameter graphene oxide by employing a secondary intercalation technique. Three different approaches were explored to control the size of the produced GO sheets. The results revealed that the completeness of the expansion graphite structure after initial intercalation significantly influenced the final GO sheet size, with more complete expansion leading to larger sheets. Optimal processing conditions were identified, involving soaking natural flake graphite in a mixed solution (H2SO4:H2O2 = 4:1), followed by drying at 60 °C for 24 h. Under these conditions, ultra-large GO sheets were predominantly monolayer with an average size of 220.99 μm and a maximum size of 438 μm. These monolayer GO sheets can be chemically reduced to graphene, making them promising for applications in transparent conductive films, optoelectronic devices, and aligned graphene composites.