Abstract: Bentonite is a natural layered clay mineral with montmorillonite as its main component. Due to its unique nanolayer structure, high specific surface area, and abundant surface hydroxyl groups, bentonite is endowed with good adsorption, hydrophilicity, cation exchange properties, heat resistance and swelling. Hence, bentonite has been proved to have significant advantages in the construction of novel gel materials. Basing on the synergistic mechanisms between bentonite and gel matrixes, this study investigates the key role of bentonite in enhancing the mechanical properties, optimizing the adsorption properties, improving the thermal stability and strengthening the ionic conduction function of gel materials. Furthermore, the applications of novel gel materials via bentonite modification in pollution adsorption, catalytic degradation, drug release, flame retardant, temperature resistance and conductive sensing are summarized. Finally, the current challenges and future development trends of bentonite in the construction of novel gel materials are analyzed. In all, this study can provide a multi-scale research perspective of bentonite in high-value utilization and the design of novel gel materials.