Nucleic acids, because of their key biological role, are prime targets for the design of either analogues that may mimic some of their features or of complementary ligands that may selectively bind to and react with them for regulation or reaction. Whereas there has been much work on the latter topic since the elucidation of the double-helical structure of DNA, comparatively little has been done on structural and/or functional models, probably owing to the lack of self-organizing molecular systems. Here we present a class of artificial systems, the nucleohelicates, which are of interest from both points of view because they combine the double-helical structure of the double-stranded metal complexes, the helicates, with the selective interaction features of nucleic-acid bases. These functionalized species allow the study of structural effects on the formation of the double helix and on the binding to other entities, in particular to nucleic acids.