Two new heterobimetallic phenylmercury(ii) dithiocarbamate complexes incorporating the ferrocenyl moiety (C(5)H(5))Fe(C(5)H(4)) (Fc), namely PhHgS(2)CN(CH(2)Fc)CH(2)C(5)H(4)N, (1) and PhHgS(2)CN(CH(2)Fc)CH(2)C(4)H(3)O, (2) have been prepared and characterized by elemental analysis, UV-Vis, IR, (1)H and (13)C NMR spectroscopies. The crystal structures of 1 and 2 showed a linear core at the Hg(ii) centre of the molecule, bound by the sulfur atom of the dithiocarbamate ligand and carbon atom of the aromatic ring. Weak intermolecular HgS interactions form "head-to-tail" dimers in the cases of 1 and 2. The observed quasi-reversible cyclic voltammograms of the complexes have been corroborated by calculating gross natural electron population and gross natural electron spin population at each atom for the neutral as well its oxidized species obtained at density functional level (DFT) of theory, which suggests that the delocalization of electron spin population can affect the magnitude of ΔE(p). The electronic absorption bands of both the complexes were assigned with the help of time dependent density functional theory (TD-DFT) calculations. The light harvesting properties of both 1 and 2 in conjunction with our previously reported compound PhHgS(2)CN(CH(2)Fc)CH(2)C(6)H(5) (3) have been reported.