Environmental pollution is a global problem that endangers human health and ecological balance. As a new type of functional material, two-dimensional material (2DM)-based aerogel is one of the most promising candidates for pollutant detection and environmental remediation. The porous, network-like, interconnected three-dimensional (3D) structure of 2DM-based aerogels can not only preserve the characteristics of the original 2DMs, but also bring many distinct physical and chemical properties to offer abundant active sites for adsorbing and combining pollutants, thereby facilitating highly efficient monitoring and treatment of hazardous pollutants. In this review, the synthesis methods of 2DM aerogels and their broad environmental applications, including various sensors, adsorbents, and photocatalysts for the detection and treatment of pollutants, are summarized and discussed. In addition, the sustainability of 2DM aerogels compared to other water purification materials, such as activated carbon, 2DMs, and other aerogels are analyzed by the Sustainability Footprint method. According to the characteristics of different 2DMs, special focuses and perspectives are given on the adsorption properties of graphene, MXene, and boron nitride aerogels, as well as the sensing and photocatalytic properties of transition metal dichalcogenide/oxide and carbon nitride aerogels. This comprehensive work introduces the synthesis, modification, and functional tailoring strategies of different 2DM aerogels, as well as their unique characteristics of adsorption, photocatalysis, and recovery, which will be useful for the readers in various fields of materials science, nanotechnology, environmental science, bioanalysis, and others.