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. Controllable synthesis of graphene is of great importance for both foundational researches and practical applications. This Progress Report summarizes recent advances in synthesizing graphene with controlled sizes, shapes, edges, layers, doping, and assembly, discusses their applications, and clarifies the problems and prospects the future development. It will be valuable for the development of research in this field.