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The natural process of photosynthesis is paradigmatic in converting sunlight into energy. This complicated process requires a cascade of energy- and electron-transfer events in a highly organised matrix of electron–donor, electron–acceptor and antennae units and has prompted researchers to emulate it. In fact, energy- and electron-transfer processes play a pivotal role in molecular-scale optoelectronics. In this chapter we compile a number of remarkable examples of noncovalent aggregates formed by the combination of carbon-based electroactive species (fullerenes and carbon nanotubes) hydrogen bonded with a variety of moieties. We will show that: (a) the connection of complementary electroactive species by means of H bonds in C60-based donor–acceptor ensembles is at least as efficient as that found in covalently connected systems; (b) hydrogen-bonding fullerene chemistry is a versatile concept to construct supramolecular polymers, and (c) H-bonding interactions is contributing to create very appealing carbon-nanotube-based donor–acceptor supramolecular architectures.

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