A complex of 2(2-pyridyl)-4,4,5,5-tetramethyl-4,5-dihydro-1H-imidazol-1-oxy-3-N-oxide (NIToPy) with Cd(II)Cl2, [(CdCl2)3-(NIToPy)2(C2H5)2], has been structurally and cryomagnetically characterized. The structure is based on a layered zigzagging polymeric chain along the (101) plane; the Cd(II) ions are linked into infinite chains by double chlorine bridges alternating between one CdCl4O2 and two CdCl4NO octahedral coordination units. The temperature-dependence of the magnetic susceptibility reveals the presence of a Heisenberg antiferromagnetic exchange interaction of a two spin Full-size image (<1 K) system, with J = −0.25 cm−1 associated with the intermolecular interaction between the NO groups of two neighboring NIToPy radicals.