In this manuscript, the structure liking a Chinese food “hemp flowers” is formed through polyphenyl which is induced by C70. The whole formation process is tracked by the molecular dynamics simulation. The results exhibited that C70 induced polyphenyl to form a “hemp flowers” structure experiencing four stages which are transfer, wrap, maintain and twist. Both the van der Waals potential well and the π–π stacking interaction between the polyphenyl and C70 play the major role in the formation of helical nanostructures. The position of C70 makes the configuration different from the “hemp flowers”. Furthermore, the final configuration of polymer is also depended on the number of C70, the length of polymer and the simulation temperature. The new geometrical structures between polyphenyl and C70 may supply more theoretical foundation in chemical functionalization and helical polymer synthesis, which may be helpful insight for fabricating nanoscale devices.