The generation, isolation, X-ray crystallographic structures, and magnetic behavior of N-(arylthio)-2-tert-butyl-4,6-diarylphenylaminyls (2) and N-(arylthio)-4-tert-butyl-2,6-diarylphenylaminyls (3) are described. Radicals 2 and 3 were generated by PbO2 oxidation of N-(arylthio)-2-tert-butyl-4,6-diarylanilines and N-(arylthio)-4-tert-butyl-2,6-diarylanilines, and seven radicals were isolated as the pure radical crystals. The X-ray crystallographic structures of N-[(4-nitrophenyl)thio]-4-tert- butyl-2,4-diphenylphenylaminyl and N-[(4-nitrophenyl)thio]-4-tert-butyl-2,6-diphenylphenylaminyl radicals were determined. The magnetic susceptibility measurements for the isolated radicals were carried out in the temperature range 1.8 - 300 K with a SQUID magnetometer. Among the four radicals studied the two were analyzed by an alternating one-dimensional Heisenberg model with J(1)/k = 1.8 (a = 0.86) and -18.2 K (a = 0.16), and the other two were analyzed by a one-dimensional regular Heisenberg model with J(1)/k = -30.8 K or a singlet-triplet dimer model with J(1)/k = -45.2 K.