A plethora of potential applications of carbon nanotubes (CNTs) have been proposed based on their unique strength, high aspect ratio and excellent thermal and electronic properties. However, difficulties in their processing and manipulation have hindered their utilisation in materials and devices. A successful strategy to improve CNT solubility and chemical attachment to other small molecules, metals, surfaces or polymers is the covalent attachment of appropriate moieties on their surface. In this direction, the synthesis of nucleobase–CNT hybrids gives the flexibility of exploiting the four different units A, C, G and T (or U) all of which offer different binding characteristics. Nucleobases not only interact with each other by the formation of hydrogen bonding, but also interact with other small organic molecules, as well as with metals. In this contribution, we focus on examples of how nucleobase–CNT hybrids have been used as building blocks to direct the self-assembly in the construction of functional CNT architectures.
