Graphene and C60 can establish coordination bonds with transition metal atoms/clusters. Using first-principles modeling methods, we explore the C60–Fen–graphene intercalating nanostructures (n=1–6), which may have potential applications in, e.g., spintronics. Twelve optimized configurations are found to possess good energetic stability (with binding energies of 4.22–20.54eV). Eleven structures have different magnitudes of magnetism (2.00–12.75μB/cell), whereas one is non-magnetic. The magnetism is highly correlated with the bonding orientations between Fe atoms and C60. Seven nanostructures possess good half metallicity (with the spin polarization effects >0.8), while the non-magnetic structure is found to be insulating.