Supramolecular Oleogel lubricants provide a versatile and reliable strategy for optimizing the long-term dispersion stability of nanoadditives in the base oils. In this work, GLM-based ionic gelators constructing supramolecular oleogels were prepared by adding ultrasonically treated gallium-based liquid metal (GLM) nanodroplets carrying free radicals and vinyl-containing ionic liquids (ILs) directly to a free radical polymerization system of polymer gelators. The electrostatic interactions between the ionic liquids and GLM nanodroplets enhanced the cross-linking degree of supramolecular gels and formed denser self-assembled structures. The as-prepared GLM-based ionic oleogels as thermoreversible gels exhibit exceptional thixotropic properties. Compared to the base oil PAO10, the coefficient of friction (COF) for both GLM@IGel-1 and GLM@IGel-2 decreased significantly from 0.192 to 0.097, while the wear volume dropped from 100.10 × 104 μm3 to 13.28 × 104 μm3 for GLM@IGel-1, and to 9.69 × 104 μm3 for GLM@IGel-2. In addition, GLM@IGel-2 demonstrates a higher load-bearing capacity of 550 N due to further chemical cross-linking by ionic liquids. The outstanding lubrication performance of GLM-based ionic oleogels is achieved by the synergy of GLM nanodroplets and gel lubricants, promoting the formation of a stable tribo-chemical reaction film.