The synthesis and full characterization (including X-ray structures) of two redox-active terpyridine-tetrathiafulvalene ligands namely (4-amido-2,2:6,2-terpyridyl)-6,7-ethylenedithiotetrathiafulvalene (1) and 2-(4-thioacetamide-2,2:6,2-terpyridyl)-3,6,7-tris(methylsulfanyl)-6, tetrathiafulvalene (2) are described. The binding properties of these multifunctional systems for various transition metal cations (Ni2+, Zn2+, Cd2+ and Fe2+) are analyzed in solution by cyclic voltammetry and UV-visible spectroscopy. In addition, a tetrahedral neutral zinc metal complex of ligand (2) formulated as (MeS)(3)-TTF-SCH2CONH-Tpy-ZnCl2 center dot MeOH [complex (3)] and an octahedral nickel complex formulated as [{(MeS)(3)-TTF-SCH2CONH-Tpy}(2)Ni]center dot(ClO4)(2)center dot 0.5(H2O) [complex (4)] are characterized in the solid state by X-ray diffraction.