Two novel ion-pair complexes, [IBzPy][Ni(Bdt)2] (I) and [IBzDMPy][Ni(Bdt)2] (II) (IBzPy = 1-(4-iodobenzyl)pyridinium, IBzDMPy = 1-(4-iodobenzyl)-3,5-dimethyl-pyridinium, and Bdt = benzene-1,2-dithiolate), have been synthesized and characterized by elemental analysis, IR, cyclic voltammetry, and X-ray single-crystal structure determination. The crystal structure determination reveals that the central Ni atoms in complexes I and II are in slightly distorted square-planar coordination environment. The cyclic voltammetric studies show that there are two oxidation peaks for complexes I and II, which are attributed to Ni(IV/III) and Ni(III/II) redox couples.