Owing to inherent 2D structure, high electrical/thermal conductivity, and superstrong mechanical properties along basal plane, [1] the promising applications of graphene are anticipated as a macroscopic thin film for coatings, [2] composites, [3] flexible electrodes, [4] sensors, [5] and so on. [6] Currently, the preparation of graphene thin film relies principally on chemical vapor deposition growth on metal surface, followed by transferring it onto desired substrate. [7] Chemical vapor deposition growth can provide large-area uniform graphene thin film. Nevertheless, vacuum processing at high temperature requires expensive and precise equipment, as well as long batch times. The transfer process is complex and often involves multiple steps, including sacrificial polymer layer immobilization, metal etching, transfer, drying, and sacrificial polymer removal. [8] An alternative strategy to prepare graphene thin film is the direct processing of graphene oxide dispersion on target substrates through conventional solution methods, [9] such as drop casting, [10] spin coating, [11] rod coating, [12] spray coating, [13] or dip coating, [14] followed by chemical reduction and/or thermal annealing. Although some of these methods might be scaled up potentially, the fabrication of graphene film with nanometer-scale control of thickness and uniformity over large area remain a challenge.With the development of solvent exfoliation techniques, it is firmly established that graphite can be directly exfoliated into large-volume, defect-free, few-layer graphene dispersion in low-volatile, polar organic solvent, such as N-methyl-2-pyrrolidone (NMP). [15] The mass exfoliation provides the premise for cost-effective production of graphene-based ultrathin film from pristine graphene. However, conventional solution processing methods are not suitable for the solvent-exfoliated graphene dispersion because of preferred aggregation in the following drying process. Therefore, further research efforts should be made to develop new processing technique that can convert solvent-exfoliated pristine graphene dispersion into macroscopic thin film on desired substrates. [16] Liquid interface provides an ideal platform for assisting in the formation of uniform thin film assembled by graphene nanoplatelets, [16a,17] delicately avoiding of graphene aggregation issue during drying dispersion. In this study, we design a robust wetting-induced climbing strategy to transfer interfacially assembled large-area ultrathin pristine graphene film. Once Owing to inherent 2D structure, marvelous mechanical, electrical, and thermal properties, graphene has great potential as a macroscopic thin film for surface coating, composite, flexible electrode, and sensor. Nevertheless, the production of large-area graphene-based thin film from pristine graphene dispersion is severely impeded by its poor solution processability. In this study, a robust wetting-induced climbing strategy is reported for transferring the interfacially assembled large-area ultrathin pri...