The new lanthanide-dicyanoaurate coordination polymers [(Bu4N)-Bu-n](2)[Ln(NO3)(4)Au(CN)(2)] (Ln = Sm, Dy) and Sm[Au(CN)(2)](3)center dot 3H(2)O were prepared and structurally characterized and their luminescence spectra described. The emissions of solid-solutions of [(Bu4N)-Bu-n](2)[Ln(NO3)(4)Au(CN)(2)] (Ln = Ce, Sm, Eu, Tb, and Dy) were explored with an emphasis on their capacity for luminescent color tuning and white-light emission via the selection of composition, excitation wavelength, and temperature. Specifically, the binary solid-solutions [(Bu4N)-Bu-n](2)[Ce0.4Dy0.6(NO3)(4)Au(CN)(2)] and [(Bu4N)-Bu-n](2)[Sm0.75Tb0.25(NO3)(4)Au(CN)(2)], and the ternary solid-solutions [(Bu4N)-Bu-n](2)[Ce0.2Sm0.6Tb0.2(NO3)(4)Au(CN)(2)] and [(Bu4N)-Bu-n](2)[Ce(0.3)3Eu(0.17)Tb(0.5)(NO3)(4)Au(CN)(2)], were prepared and examined in terms of suitability for color-tuning capacity. These results [(Bu4N)-Bu-n](2)[Ln(NO3)(4)Au(CN)(2)] framework has the capacity to be tuned to extremes corresponding to deep reds (CIE coordinates 0.65, 0.35), greens (0.28, 0.63), and deep blue/violet (0.16, 0.06) as well as white (0.31, 0.33). Conversely, the emission of the Sm[Au(CN)(2)](3)center dot 3H(2)O framework, when doped with the green phosphor Tb(III), changes only slightly because of the predominantly Au(I)-based emission and Sm(III) -> Au(I) energy transfer.