In this study, in order to obtain polymeric thiourea compounds which have unsolubulity properties and higher metal content, new reaction pathways based on the use of the template effect were investigated. For this purpose, the reactions between different diamines, such as ethylendiamine, ortho (o-) and para (p-) phenylenediamine, and carbon disulfide (CS 2 ) were investigated and optimized by using the template effect of Ni(II). Catalytic activity of the polymeric structure on oxidation of styrene was also investigated in terms of different parameters such as heat (25 and 80 • C), time (4 and 8 h), oxidant hydrogen peroxide (H 2 O 2 ), tert-butyl hydroperoxide (TBHP), di-tert-butyl peroxide (DtBP) and solvent (acetonitrile and benzene). The products have been characterized on the basis of analytical and spectral method, Fourier transform infrared spectroscopy, 1 H-and 13 C-nuclear magnetic resonance, gel-permeation chromatography, elemental analysis, thermogravimetric analysis, atomic adsorbtion spectrometry, gas chromatography and gas chromatography mass spectrometry.