Predictive catalysis must be the tool that does not replace experiments, but acts as a selective agent, so that synthetic strategies of maximum profitability are used in the laboratory in a surgical way. Here, nanotechnology has been used in olefin metathesis from homogeneous Ru‐NHC catalysts, specifically annulating a C60 fullerene to the NHC ligand. Based on results with the C60 in the backbone, a sterile change with respect to the catalysis of the metal center, an attempt has been made to bring C60 closer to the metal, by attaching it to one of the two C−N bonds of the imidazole group of the SIMes (1,3‐bis(2,4,6‐trimethylphenyl)imidazolin‐2‐ylidene) ligand (reference NHC ligand of the 2nd generation Grubbs catalysts) to increase the steric pressure of C60 in the first sphere of reactivity of the metal. The DFT calculated thermodynamics and the kinetics of SIMes‐derived systems show that they are efficient catalysts for olefin metathesis. Annulating C60 fullerenes in NHC ligands enhances the catalysis of Ru‐based olefin metathesis catalysis.