▎ 摘　　要

Graphene, the strongest, stiffest, and most conductive material known to date, would enable very strong, stiff, and highly conductive materials that would be better than what is available currently. These would be useful in a variety of fields, particularly flexible electronics and aerospace. Thus, to realize this potential, it is necessary to transfer these remarkable properties from graphene nanosheets into macroscopic graphene films. Nacre provides an inspiration for assembling graphene nanosheets into high-performance graphene films by constructing abundant interfacial interactions and a highly aligned structure. However, several issues in the assembly process, including intersheet bonding, dewrinkling, and alignment of graphene nanosheets, have been ignored in descriptions of previously reported macroscopic graphene films. This Review clarifies and compares the interface architecture of macroscopic graphene films described in previous reports. The representative orientation strategies are then summarized and the relationship between alignment and properties is discussed. Finally, perspectives and challenges are proposed to highlight the guidelines on how to construct high-performance graphene films in the future.