A process of forming a nanopatterned substrate is provided. The process comprising the steps of first preparing a giant surfactant comprising a cage-like molecular nanoparticle head linked to a polymer chain tail through a chemical linkage. Next, using the giant surfactant, a thin film is formed. Next the thin film formed from the giant surfactant is annealed such that the giant surfactant self-assembles into a desired nanostructure. The desired nanostructure is comprised of periodic major domains and minor domains. Finally, at least some of either the major domain or the minor domain is selectively removed to form the nanopatterned substrate.