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An RNA-based coordination polymer is formed by the aqueous reaction of Cu I ions with the thionucleoside enantiomer (-)6-thioguanosine, (6tGH). The resulting polymer, [Cu I (μ 3 -S-thioG)] n 1, has a one-dimensional structure based on a [Cu 4 -S 4 ] core and undergoes extensive hierarchical self-assembly transforming from oligomeric chains → rod → cable → bundle through which a fibrous gel forms, that undergoes syneresis to form a self-supporting mass. The assembly involves the formation of helical cables/bundles and, in combination with the intrinsic photoemission of the polymer, results in the material exhibiting circularly polarised luminescence (CPL).