Supramolecular nanostructures (SNSs) have received significant attention in recent years since they endow specific and unique properties to materials. Pillararenes, as a novel group of macrocyclic molecules, present particular features such as ease of modification, more electron-rich cavity as well as captivating host-guest chemistry, thus bestowing them with the abilities to fabricate intriguing SNSs. This feature article highlights the construction methods of pillararene-based supramolecular nanostructures (PSNSs), where most of which are in aqueous media, and the factors that influence the morphological transformation of PSNSs. Moreover, the structure-function relationship of divergent PSNSs is clarified. Finally, the future challenges and perspectives for PSNSs are pointed out and discussed. We hope this review will benefit the researchers interested in engineering PSNSs with on demand morphologies and desired functions.