Recent development of artificial photosynthetic systems using photofunctional nanomaterials composed of multiporphyrins and carbon-based π-electron acceptors such as fullerenes, carbon nanotubes and a new type of nanocarbon is reviewed by focusing on their photoinduced electron-transfer properties. Electron donor–acceptor ensembles composed of porphyrins and fullerenes are described, covering small electron donor–acceptor dyads to larger multi-component systems including porphyrin-based photofunctional nanometerials. Such photofunctional nanomaterials composed of multiporphyrins and carbon-based π-electron acceptors (in particular C60) have been utilized to construct efficient light energy conversion systems such as photovoltaic devices.