The graphene nanoparticles incorporated in thin polystyrene film in different configurations, garner into unique phenomenon of self-assembly regulated by the self-organization of the thin polystyrene film. The polystyrene–graphene nanoparticles composite when spin-coated together to form a thin film over a substrate, was observed to self-assemble in a Voronoi tessellation of ribbon-like structure. The suppression of dewetting of thin polystyrene film at the stage, where the holes coalesce and grow to form Voronoi tessellation of polymeric ribbons, sways the path for the graphene nanoparticles to self-assemble and organize into a Voronoi tessellation-like pattern of graphene nanoparticles. In the second method, the graphene nanoparticles dispersed in solvent were casted over the instability based dewetting patterns formed on the surface of the thin polystyrene film. This method exclusively caused the graphene nanoparticles to arrange in a polygonal array of dots prompted by the dynamics and morphology of dewetting. The reversals of the dewetted patterns were observed in this process, because of the solvent evaporation and Marangoni flow. The graphene nanoparticles in the presence of solvent destruct and self-healed the dewetted holes formed on the surface of the pure polystyrene thin film.