Two cationic derivatives of alpha-nitronyl nitroxide (NN), p-PPYNN (p-N-n-propylpyridinium alpha-nitronyl nitroxide) and p-BPYNN (p-N-n-butylpyridinium alpha-nitronyl nitroxide), have been crystallized with the [Co(Pc)(CN)2](-) (dicyanophthalocyaninatocobalt(III)) counter anion. Obtained two kinds of 1:1 salt crystals have been found to be isomorphous; monoclinic, P2(1)/c, a = 15.585(6), b = 11.015(4), c = 26.111(3) Angstrom, beta = 89.95(2)degrees, V = 4482(3) Angstrom(3), Z = 4 for p-PPYNN[Co(Pc)(CN)(2)] and a = 15.830(3), b = 11.201(4), c = 25.709(3) Angstrom, beta = 90.29(1)degrees, V = 4558.4(17) Angstrom(3), Z = 4 for p-BPYNN[Co(Pc)(CN)(2)]. The magnetic interaction between the NN radicals in these two kinds of crystals has been found not to be the same; weak antiferromagnetic interaction operates in p-PPYNN[Co(Pc)(CN)(2)], while only paramagnetic behavior is observed for p-BPYNN[Co(Pc)(CN)(2)].