The present review highlights the recent progresses in the preparation of supramolecular, donor–acceptor (D–A) porphyrin (Por)- and phthalocyanine (Pc)/carbon nanostructure systems assembled by using noncovalent interactions such as hydrogen bonding, metal–ligand, cation-crown ether or π–π interactions. The use of supramolecular interactions as a tool to promote the nanoscopic order of covalently-linked, Por- or Pc–C60 fullerene systems over large length scales will also be reviewed. The photophysical analysis of most of the D–A, supramolecular ensembles described will also be presented with the aim of rationalizing the effect on the photoinduced electron/energy-transfer dynamics of the structural and electronic features of these self-assembled systems and the recognition motif(s) used to self-assemble them. For some of the supramolecular systems reviewed, their incorporation as active components in photovoltaic devices will also be discussed.