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Based on this concept, fabrications of functional materials with hierarchical structural motifs from simple nano units of fullerenes (C60 and C70 molecules) are described in this review article. Because fullerenes can be regarded as simple and fundamental building blocks with mono-elemental and zero-dimensional natures, these demonstrations for hierarchical functional structures impress the high capability of the nanoarchitectonics approaches. In fact, various hierarchical structures such as cubes with nanorods, hole-in-cube assemblies, face-selectively etched assemblies, and microstructures with mesoporous frameworks are fabricated by easy fabrication protocols. 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