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The well-established exohedral functionalization chemistry of fullerenes, with C 60 as the most prevalent example, provides easy access to a variety of functionalized carbon nanostructures with great structural diversity and unusual spatial orientation of the attached moieties. Therefore, such molecular nanostructures can be identified as promising building blocks for the design and synthesis of three-dimensionally cross-linked molecular architectures giving rise to novel topologies which would not be accessible from other organic building blocks. Within this perspective, we would like to give an overview on recent progress in the design and synthesis of metal–organic hybrid architectures composed of highly functionalized fullerene derivatives as organic connectivity centers and metal ions or clusters as cross-linking nodes. The ultimate goal of these investigations is the precise control of three-dimensional arrangements of fullerene units in the solid state and the implementation of such carbon derivatives as organic connectivity centers into porous functional materials such as metal–organic frameworks (MOFs). [ABSTRACT FROM AUTHOR]