Graphene, an individual two-dimensional, atomically thick sheet of graphite composed of a hexagonal network of sp2 carbon atoms, has been intensively investigated since its first isolation in 2004, which was based on repeated peeling of highly oriented pyrolyzed graphite (HOPG). The extraordinary electronic, thermal, and mechanical properties of graphene make it a promising candidate for practical applications in electronics, sensing, catalysis, energy storage, conversion, etc. Both the theoretical and experimental studies proved that the properties of graphene are mainly dependent on their geometric structures. Precise control over graphene synthesis is therefore crucial for probing their fundamental physical properties and introduction in promising applications. In this Minireview, we highlight the recent progress that has led to the successful chemical synthesis of graphene with a range of different sizes and chemical compositions based on both top-down and bottom-up strategies.