Controlled Growth of Single‐Crystal Graphene Films

Abstract Grain boundaries produced during material synthesis affect both the intrinsic properties of materials and their potential for high‐end applications. This effect is commonly observed in graphene film grown using chemical vapor deposition and therefore caused intense interest in controlled growth of grain‐boundary‐free graphene single crystals in the past ten years. The main methods for enlarging graphene domain size and reducing graphene grain boundary density are classified into single‐seed and multiseed approaches, wherein reduction of nucleation density and alignment of nucleation orientation are respectively realized in the nucleation stage. On this basis, detailed synthesis strategies, corresponding mechanisms, and key parameters in the representative methods of these two approaches are separately reviewed, with the aim of providing comprehensive knowledge and a snapshot of the latest status of controlled growth of single‐crystal graphene films. Finally, perspectives on opportunities and challenges in synthesizing large‐area single‐crystal graphene films are discussed.