Just as graphene triggered a new gold rush, three-dimensional graphene-based macrostructures (3D GBM) have been recognized as one of the most promising strategies for bottom-up nanotechnology and become one of the most active research fields during the last four years. In general, the basic structural features of 3D GBM, including its large surface area, which enhances the opportunity to contact pollutants, and its well-defined porous structure, which facilitates the diffusion of pollutant molecules into the 3D structure, enable 3D GBM to be an ideal material for pollutant management due to its excellent capabilities and easy recyclability. This review aims to describe the environmental applications and mechanisms of 3D GBM and provide perspective. Thus, the excellent performance of 3D GBM in environmental pollutant adsorption, transformation and detection are reviewed. Based on the structures and properties of 3D GBM, the removal mechanisms for dyes, oils, organic solvents, heavy metals, and gas pollutants are highlighted. We attempt to establish "structure-property-application" relationships for environmental pollution management using 3D GBM. Approaches involving tunable synthesis and decoration to regulate the micro-, meso-, and macro-structure and the active sites are also reviewed. The high selectivity, fast rate, convenient management, device applications and recycling utilization of 3D GBM are also emphasized.