Two coordination compounds of compositions [Ni(L 1 )(idba)(H 2 O)]·1.5 H 2 O (1) and [Ni(L 2 )Fe(CN) 5 NO]· C 2 H 5 OH (2) where L 1 is N, N -bis(3-aminopropyl)ethylenediamine, L 2 is 2, 12-dimethyl-3,7,11,17-tetraazabicyclo [11.3.1]heptadeca-1(17),2,11,13,15-pentaene, and idba 2− is 2,2 -iminodibenzoate have been synthesized and characterized by elemental analysis, IR spectroscopy, thermal analysis, and single-crystal X-ray diffraction. Complex 1 crystallizes in the monoclinic space group P2 1 /n (No. 14) with a = 9.810(2) Å, b = 10.230(2) Å, c = 25.350(5) Å, V = 2543.6(9) Å 3 , Z = 4, and R = 0.0727. The nickel atom is six-coordinated by four N atoms of amine and two O atoms of water and idba 2− . The molecular packing of the complex comprises of an infinite one-dimensional layered network in which the molecules in the crystal are held together by a system of hydrogen bonding. Complex 2, however, crystallizes in the space group C2/c (No. 15) of the monoclinic system with a = 19.7990(4) Å, b = 14.9440(3) Å, c = 19.8800(3) Å, V = 5115.90(17) Å 3 , Z = 4, and R = 0.0540. The Ni ion in compound 2 has a slightly distorted octahedral arrangement of the N 4 donor atoms of primary ligand L 2 and two N-donor atoms of the secondary nitroprusside ligand. The structure of 2 displays an extended one-dimensional network formed by linear [ Ni NC Fe CN ] units. A cyclic voltammetric study shows that compound 1 undergoes a quasireversible oxidation attributable to Ni 2+ → Ni 3+ in the range 300-420 mV vs SCE.