Guanosine and isoguanosine derivatives can self-assemble by means of hydrogen-bonding, π–π and cation–dipole interactions, yielding supramolecules that have found broad applications in diverse areas, such as material science, medicinal chemistry or nanotechnology. This article reviews the different self-organized architectures generated by guanosine and isoguanosine scaffolds and reports on recent examples of their use in the preparation of functional devices.