Host-guest supramolecular complexes formed by molecular interactions, in which various guest molecules are accommodated in crack, cavity, or cage of host compounds, have made great contributions to the development of advanced functional materials. One of the most prominent examples of host-guest system is the binding of host and guest molecules through non-covalent interactions between complementary convex-concave surfaces. Traditionally, fullerenes C 60 and C 70 have long been studied as guests in various organic architectures due to their unusual spherical structure, and the cycloparaphenylenes (CPPs) were usually served as excellent cyclic hosts for encapsulation. So far, C 60 @CPPs and C 70 @CPPs have attracted enough attention with their fascinating topologies. Over the past few years, organic macrocycles with twisted π-conjugation have become the focus of materials chemists on account of their exceptional structures and interesting functionalities. They typically have unique nanoscale cavities that can be used for supramolecular assembly. Very recently, a special oligoparaphenylene nanohoop (referred to as OPP in the following) was successfully synthesized by employing cyclooctatetrathiophene as a linker to connect two [10]paraphenylene loops. Different from most conjugated monocycles, the newly prepared OPP is a dual-loop nanohoop with a figure-eight configuration. What makes this macrocycle especially intriguing is that its two loops can each accommodate a molecule, such as fullerene C 60 or C 70 , through non-covalent interactions to form a dual-guest supramolecular complex, which has been confirmed by X-ray crystallographic analyses of its synthetic experimental group.