This review presents recent progress concerning the organization of nucleobases on highly ordered pyrolytic graphite (HOPG), mica, Cu(110) and Au(111) surfaces, followed by their studies using microscopy methods such as atomic force microscopy (AFM), scanning tunneling microscopy (STM) and transmission electron microscopy (TEM). Interesting research prospects related to surface patterning by nucleobases, nucleobase-functionalized carbon nanotubes (CNTs) and metal-nucleobase coordination polymers are also discussed, which offer a wide array of functional molecules for advanced applications. Nucleobases and their analogs are able to invoke non-covalent interactions such as p-p stacking and hydrogen bonding, and possess the required framework to coordinate metal ions, giving rise to fascinating supramolecular architectures. The latter could be transferred to conductive substrates, such as HOPG and gold, for assessment by high-end tunneling microscopy under various conditions. Clear understanding of the principles governing nucleobase self-assembly and metal ion complexation, and precise control over generation of functional architectures, might lead to custom assemblies for targeted nanotechnological and nanomaterial applications.