Template reactions of 2,4-dihydroxy-, 2,5-dihydroxy-, 2-hydroxy-3-methoxy- and 2-hydroxy-4-methoxy-benzalde-hyde with methoxy- and hydroxy-substituted salicylaldehyde S-methylthiosemicarbazones in the presence of NiCl2 and FeCl3 resulted in the corresponding hydroxy- and methoxy-substituted N-1,N-4-diarylidene-S-methylthiosemi-carbazone complexes. Characterization of the compounds, [Fe(L)Cl] and [Ni(L)], was accomplished by means of elemental analysis, conductivity and magnetic measurements, i.r. and H-1-n.m.r. spectra. A systematic trend has been observed for the chemical shift values of the aromatic protons in the spectra of complexes.