Montmorillonite (MMT) aerogels with many excellent physicochemical properties of low density, high surface area, thermal stability and adjustable surface chemistry have been found as a new class of functional aerogels. Recently, MMT aerogels have aroused wide attention as the adsorbent for the removal of various pollutants posing a hazard to the environment and human health. However, MMT aerogels got limited in environmental remediation due to their poor mechanical properties and limited adsorption capacity. Numerous efforts have been done in the past few years with the aim to improve the mechanical properties and adsorption capacity of MMT aerogels. Here, we initially summarized and discussed the preparation and properties of MMT-based aerogels, including MMT-cellulose hybrid aerogels, MMT-chitosan hybrid aerogels, MMT-synthetic polymers hybrid aerogels, as well as MMT-graphene hybrid aerogels. Particularly, the applications of MMT-based aerogels in environmental remediation including CO2 capture, adsorption of oil and toxic organic compounds, dyes and heavy metal ions are analyzed in detail. Finally, the existing and future challenges of such materials are described to guide researchers to catch up with new opportunities in this promising field. This review summarized recent progresses in the preparation of montmorillonite (MMT)-based aerogels and their applications in environmental remediation. Display omitted