N-[(4-Nitrophenyl)thio]- (1a) and N-[(2,4-dichlorophenyl)thio)]-2,6-diphenyl-4-(3-pyridyl)phenylaminyl (1b), N-[(4-nitrophenyl)thio]- (2a) and N-[(2,4-dichlorophenyl)thio]-4-phenyl-2,6-di(3-pyridyl)phenylaminyl (2b) were generated by PbO2 oxidation of the corresponding precursors and isolated as radical crystals. For 1b X-ray crystallographic analysis was performed. The magnetic susceptibility measurements were carried out for the isolated radicals using a SQUID magnetometer in the temperature range 1.8 − 300 K. The susceptibilities of 1a and 2a were analyzed in terms of a one-dimensional (1D) antiferromagnetic (AFM) regular Heisenberg model with exchange interaction of 2J/k B= −63.4 and −17.8 K, respectively, and that of 1b was interpreted in terms of a 1D AFM alternating Heisenberg model with 2J/k B = −12.8 K and α = 0.91. On the other hand, that of 2b was explained in terms of a 1D ferromagnetic regular Heisenberg model with 2J/k B = 22.4 K.