Nucleobases are nitrogenous heterocyclic compounds and have high ability to form directionally controlled multiple intermolecular interaction, i.e., in-plane multiple hydrogen-bonding interactions and stacking interactions perpendicular to the plane. Here the recent development of nucleobase-containing low molecular mass gelators in aqueous and organic systems is reviewed, and the self-assemblies of nucleobase-containing small molecules and their arrangement within the gel are discussed from the molecular, and mesoscopic to the macroscopic level in regard to becoming a macroscale three-dimensional network. Brief overview of the nucleoside-containing supramolecular materials are also presented.