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Carbon nanotubes, fullerenes and graphene are typical examples of extensively used nanocarbons in materials sciences due to their excellent electronic and mechanical properties. Different from 1D carbon nanotubes and 2D graphene, fullerene has a special spherical geometry, rich electrochemistry and is soluble in several solvents. It has also been found that the performance of fullerene-based device is related to its morphology. As a consequence, controlled fabrication of various supramolecular architectures of fullerene (C₆₀) through self-assembly has received much attention. Usually, a large bulky substituent such as long alkyl chain was attached on surface of C₆₀ cage to obtain complex morphology, whereas the C₆₀ content in final architecture was seriously decreased. In this presentation, series small substituent functionalized C₆₀ was designed and their electrochemistry, self-assembly as well as potential application in electrocatalyst support for methanol oxidation reaction will be presented. The results showed that there was a linear relationship between the first reduction potentials of fullerene derivatives and the substituent constants; flowerlike architectures were facilely constructed and an enhanced electrocatalytic activity and durability in methanol oxidation reaction were also observed.