Functional assemblies of inorganic nanoparticles (NPs) are widely studied owing to their collective electromagnetic properties and various application from nanodrugs and bioimaging. In most cases, the superstructures of NPs are prepared with the assistance of templates or external fields. Therefore, how to prepare the functional assemblies of NPs more simply remains a challenge. Here, a free-template assembly strategy for preparing the superstructures of NPs is proposed in our work. In our strategy, we design poly(glycerol monomethacrylate)-b-poly(2-hydroxypropyl methacrylate) (PGMA-b-PHPMA) coated NPs. Then, using the polymerization-induced self-assembly (PISA), hydrophobic PHPMA blocks resulted in the phase separation to form the orderly patterns, which is expected to induced NPs to self-assemble into the orderly superstructures. By DPD simulations, we find that the disk, ring, composite superstructures can be obtained by regulating the graft density, verifying that our assembly strategy of NPs is feasible. Even more interesting is that NPs are also distributed in an orderly way on the surface of aggregations to form the orderly NP patterns. Besides that, the thermodynamics, dynamics, and structure details in the self-assembly process of HINPs are shown in our work, providing a new idea and elaborate physical picture for the following preparation of the superstructure of NPs.