The objective of this work is to synthesize closely-spaced disordered nanocomposites of cobalt for producing μm-thick films of non-conductive ferromagnet with high moment . Commercial graphene-coated nanoparticles (Co/C) are used since graphene prevents metallic core from oxidation (i .e . saturation magnetization of 150emu/g). Synthesis of nanocomposites is based on two original functionalization schemes. First Co/C are functionalized by non-covalently grafting low molecular weight pyrene-terminated polystyrene (Pyr-PS 1 ) on graphene to obtain Co/C//PyrPS 1 product . Second Co/C//PS 1 is produced by covalent in situ polymerization of styrene monomers . As a result, uniform outer-shell successfully forms (2-4nm thick) around the nanoparticles of Co/C and avoids electric percolation while promoting strong dipolar coupling at room temperature . Thereby, we report that core double-shell particles of Co/C//Pyr-PS 1 or Co/C//PS 1 assembled in closely-spaced arrangements are strong enough to sustain different magnetic orders (antiferromagnetic, ferromagnetic, “amorphous-like”) both in cast solutions and films . At the end, a second high molecular weight polystyrene PS 2 is used as an encapsulating matrix to form Co/C//Pyr-PS 1 /PS 2 or Co/C//PS 1 /PS 2 final product suitable for spin coating .