This review article highlights the recent progress made in the design and study of self-assembled supramolecular architectures based on tetrapyrrole macrocycles as donors, and fullerene and carbon nanotubes as electron acceptors for electron and energy transfer applications in solution. The remarkable features of the utilized biomimetic organization principles viz., hydrogen bonding, π–π stacking, metal-mediated complexation, and electrostatic attraction in governing the stability and geometry of the nanohybrids, and their significance in controlling the structure and electron transfer properties are discussed.