Abstract A series of novel substituted N, N'-di (arylaminothiocarbonyl) terephthalamide and 1, 4-di (aryloylthioureido) benzene were synthesized by the reaction of terephthaloyl dichloride, ammonium thiocyanate and primary amines, 1, 4-phenylenediamine and acyl halide derivatives. The reaction has been completed within 0.5 h in solvent-free condition by grinding the mixture of reactants and afforded the substituted thiourea in good yields.