Abstract: | ZnCl2(NIT‐pPy) 1 , (NIT‐pPy = 2‐(4‐pyridyl)‐4,4,5,5‐tetramethyl‐4,5‐dihydro‐1H‐imidazolyl‐1‐oxyl‐3‐oxide) crystallizes in the orthorhombic space group Pnn2 with the cell parameters a = 9.4083(9), b = 39.686(3), c = 7.4417(14) Å. ZnCl2(NIT‐6M‐oPy) 2 , (NIT‐6M‐oPy = 2‐(6‐methyl‐2‐pyridyl)‐4,4,5,5‐tetramethyl‐4,5‐dihydro‐1H‐imidazolyl‐1‐oxyl‐3‐oxide) crystallizes in the monoclinic space group Pn with a = 7.377(2), b = 19.096(4), c = 11.853(2) Å, β = 95.65(3)°. The temperature dependence magnetic susceptibility of complex 1 revealed an intermolecular ferromagnetic exchange interaction. A simple spin‐polarization model has been used to justify the observed ferromagnetic exchange interaction between the spins of the radical NO group in complex 2 . |