Giant surfactants have been identified as good candidates to produce sub-10 nm elaborate nanostructures, which could potentially realize complex functions in nanofabrication fields. Our theoretical simulation demonstrates the formation of open layered (pupa-like micelles) and closed layered (onion-like micelles) nanostructures, self-assembled from giant surfactants with comparably sized hydrophilic heads tethered by oligomers in solution. Directed by these simulation results, we synthesized giant surfactants consisting of hydrophilic [60]fullerene heads and oligostyrene (OS7) tails and produced the predicted nanostructures with periods of 9.5, 8.3, and 7.5 nm, experimentally. Adjusting the polarity of the solvent and corresponding concentration changed the nanostructures from onion-like micelles with closed layers to pupa-like micelles with open layers. The different morphologies and periods were caused by solvent inclusion and the overlap of OS chains. The above layered nanostructures remained stable after annealing at 120 degrees C. This work provides insights that computer simulation can play an important role in assisting the design and construction of complicated nanostructures in giant surfactant systems.