Supramolecular gels are physically cross-linked hydrogels formed by non-covalent interactions. The synthesis, structure optimization, property regulation, and application expansion of supramolecular gels has gradually become the research hotspot in the field of gel materials. According to the non-covalent interactions such as hydrophobic association and hydrogen bonding, the supramolecular gel prepared in this study has excellent rheological properties and adaptive filling and plugging properties, and can be used in the field of drilling fluid plugging. In this paper, the microstructure, rheological properties, temperature resistance, and plugging properties of supramolecular gels were studied and characterized in detail. The experimental findings demonstrated that when the strain was less than 10%, the supramolecular gel displayed an excellent linear viscoelastic region. The increase in strain weakens the rheological properties of supramolecular gel and reduces the elastic modulus of supramolecular gel to a certain extent. The supramolecular gel still had a neat three-dimensional reticular structure after curing at high temperatures, and the network of each layer was closely connected. Its extensibility and tensile properties were good, and it had excellent temperature resistance and mechanical strength. The supramolecular gel had excellent tensile and compressive properties and good deformation recovery properties. When the elongation of the supramolecular gel reached 300%, the tensile stress was 2.33 MPa. When the compression ratio of supramolecular gel was 91.2%, the compressive stress could reach 4.78 MPa. The supramolecular gel could show an excellent plugging effect on complex loss layers with different fracture pore sizes, the plugging success rate could reach more than 90%, and the plugging layer could withstand 6.3 MPa external pressure. The smart plugging fluid prepared with supramolecular gel material could quickly form a fine barrier layer on the rock surface of the reservoir. It could effectively isolate drilling fluid from entering the reservoir and reduce the adverse effects, such as permeability reduction caused by drilling fluid entering the reservoir, so as to achieve the purpose of reservoir protection.