Dieser Beitrag ist mit Zustimmung des Rechteinhabers aufgrund einer (DFG geförderten) Allianz- bzw. Nationallizenz frei zugänglich. ; This publication is with permission of the rights owner freely accessible due to an Alliance licence and a national licence (funded by the DFG, German Research Foundation) respectively. ; Taking advantage of the non-covalent interaction between alkyl chains and the sidewalls of a single-walled carbon nanotube (SWCNT), a nanocarbon hybrid of SWCNT and a fullerene (C60) derivative with long alkyl chains was constructed as a donor–acceptor pair for photovoltaics and nanodevice investigations. It was found that SWCNT could be mostly unbundled by the alkylated C60 (1) and was well-dispersed in organic solvents. As a photoactive material, the resultant nanocarbon hybrid, 1-SWCNT, performed well in light-energy harvesting applications in photoelectrochemical cells and nanoscale field-effect transistors (FET). Moreover, the 1-SWCNT assembly exhibited superhydrophobicity, providing an interesting opportunity to fabricate nanocarbon-based waterproof optoelectronic devices. In order to understand the photoexcitation process, the 1-SWCNT assembly was electrochemically and spectroscopically characterized. The electrochemical results showed that the SWCNT facilitated electronic communication between 1 and the electrode. The steady-state and time-resolved fluorescence and the photoluminescence excitation studies suggested efficient quenching of the singlet excited state of C60. Nanosecond transient absorption data revealed the one-electron reduction of fullerene, C60˙−, thereby demonstrating the photoinduced electron transfer from SWCNT to the C60 unit in the 1-SWCNT assembly. ; DFG, EXC 314, Unifying Concepts in Catalysis