Graphene, a two-dimensional material, is regarded as one of the most promising candidates for future nanoelectronics due to its atomic thickness, excellent properties and widespread applications. As the first step to investigate its properties and finally to realize the practical applications, graphene must be synthesized in a controllable manner. Thus, controllable synthesis is of great significance, and received more and more attention recently. This Progress Report highlights recent advances in controllable synthesis of graphene, clarifies the problems, and prospects the future development in this field. The applications of the controllable synthesis are also discussed.