 Abstract graphene oxide, GO, a one-atom-thick carbon-based nanomaterial with unique 2D-layered structure, has been significantly developed and investigated in the past decade for its potential to develop functional interfacial materials with promising performances, including large area interfacial membranes, self-healing geobased coatings, and functional geobased emulsions. The interfacial assembly behaviors of GO and functionalized GO at air-liquid, liquid-liquid, and liquid-solid interfaces are discussed to further understand the properties and applications of GO. The synthesis of different composites using these interfacial properties is also discussed, and possible challenges are proposed. This article was authored by Heng Linli, Shaoqing Shui, Yajua Shang, and others.