Polymer gels have been widely used in the field for tissue engineering, sensing, and drug delivery due to their excellent biocompatibility, hydrophilicity, and degradability. However, common polymer gels are easily deformed on account of their relatively weak mechanical properties, thereby hindering their application fields, as well as shortening their service life. The incorporation of reversible non-covalent bonds is capable of improving the mechanical properties of polymer gels. Thus, here, a poly(methyl methacrylate) polymer network was prepared by introducing host–guest interactions between pillar[5]arene and pyridine cation. Owing to the incorporated host–guest interactions, the modified polymer gels exhibited extraordinary mechanical properties according to the results of the tensile tests. In addition, the influence of the host–guest interaction on the mechanical properties of the gels was also proved by rheological experiments and swelling experiments.