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Molecular gels, which are soft and flexible materials, are candidates for healthcare, cosmetic base, and electronic applications as new materials. In this study, a new polymeric organogelator bearing a polyrotaxane (PR) structure was developed and could induce the gelation of N′,N″-dimethylformamide (DMF), a known solvent for dissolving polymeric materials and salts. Furthermore, the resulting DMF molecular gels exhibited thixotropic properties, observed by the inversion method using vials, which are essential for gel spreading. The scanning electron microscopy of the xerogels suggested that the gel-forming ability and thixotropic property of gels were imparted by the network of the laminated aggregates of thin layer material similar to those of other gels made of clay materials. This thin layer material would be formed by the aggregation of polymeric organogelators. The dynamic viscoelasticity measurements of the obtained gels revealed the stability and pseudo-thixotropic behaviors of the obtained gels, as well as a specific concentration effect on the mechanical behavior of the gels attributed to the introduction of the PR structure. Additionally, the preparation of the polymer organogelator/polymer composites was investigated to improve the mechanical properties via the filler effect induced by the agglomerates of organogelator. Moreover, the tensile tests confirmed that the introduction of the gelator enhanced the mechanical properties of the composites.