Oxidation of graphite produces graphite oxide and/or graphene oxide, both of which are abbreviated “GO”. The preparation methods of these materials have been described by Brodie, Staudenmaier, and Hummers. Graphene oxide is widely recognized as a promising material in various fields, but its structure and composition has still not been fully controlled. In this article, general strategies to control the structure, particle size, and oxidation degree of graphene-like materials are introduced with emphasis on the oxidation of graphite by KMnO4 in H2SO4 (oGO) and the reduction of highly oxidized graphene oxide by hydrazine (rGO). Even though the oxygen content is the same, oGO and rGO have different properties, such as adsorption ability, oxidation ability, and electronic conductivity, because of differences in the persisting graphitic structure and defects. These results can be used as a guideline for the production of tailor-made GO. The current method of GO preparation is also discussed.