The grafting of copolymers containing vinyl ferrocene (Vf) moieties, such as copolymer of Vf with methyl methacrylate [poly(Vf-co-MMA)] or styrene [poly (Vf-co-St)], onto the surface of nanocarbons, such as graphitized micro diamond (GpD) and carbon nanotube (CNT), was successfully carried out by ligand-exchange reaction of ferrocene moieties of these copolymers with graphene structure of GpD and CNT in the presence of AlCl₃ and Al powder as catalysts. The grafting of the copolymers onto these nanocarbons was confirmed by FT-IR, thermal decomposition gas chromatograph/mass spectra (GC/MS), and scanning electron microscope (SEM). The percentage of grafting of poly(Vf-co-MMA) onto GpD and CNT was determined to be 32.2% and 28.4%, respectively. Then, the immobilization of CNT on the surface of GpD by the reaction of poly(Vf-co-MMA)-grafted CNT [CNT-g-poly (Vf-co-MMA)], previously prepared, with GpD in the presence of the catalysts was examined. As a result, CNT was immobilized (grafted) on the GpD surface to give GpD decorated with CNT (CNT@GpD (1)). In addition, CNT@GpD (2) was obtained by the ligand-exchange reaction of GpD-g-poly(Vf-co-MMA) with CNT. CNT@GpD (3) was prepared by one-step ligand-exchange reaction in the coexistence of poly(Vf-co-MMA), GpD, and CNT, in the presence of the catalysts. The amount of immobilized CNT on CNT@GpD (1), CNT@GpD (2), and CNT@GpD (3) was determined to be 40 wt%, 55 wt%, and 14 wt%, respectively, by thermogravimetric analysis (TGA). In addition, the immobilization of CNT onto carbon micro beads (CNT@CMB) and carbon fiber (CNT@CF) was also achieved by the use of the same ligand-exchange reaction of poly(Vf-co-MMA). The silica nanoparticle-immobilized CMB and CF (Silica@CMB and Silica@CF) was obtained by the ligand-exchange reaction of Silica-g-poly(Vf-co-MMA), which was prepared by the radical graft copolymerization of Vf with MMA initiated by azo groups introduced onto the surface, with CF and CMB.