The well-directed synthesis of cadmium sulphide from aqueous solutions of its coordination compounds with a thiourea (SC(NH2)2, thio) allows to prepare the thin films, which have consisted of one or two polymorphic modifications (zinc blende or wurtzite). The technique of thermal destruction of thiourea coordination compounds by sputtering of aqueous solutions on the hot substrates has been employed in this work. The main purpose of this study is to discuss the experimental results, which have been received during the examination of the real crystal structure of CdS thin films. CdS films were fabricated from aqueous solutions of cationic [Cd(thio)4]2+ and neutral [Cd(thio)2X2] (X – Cl-, Br-, I-, and СH3COO-) complexes. The X-ray analysis data show that CdS films prepared from aqueous solutions of [Cd(thio)2(СH3COO)2], [Cd(thio)4](NO3)2, and [Cd(thio)4]SO4 complexes are characterized by zinc blende crystal structure. Under the same experimental conditions (concentration of solution and temperature of substrate) CdS layers fabricated from aqueous solutions of [Cd(thio)2Cl2] and [Cd(thio)2Br2] coordination compounds are crystallized in wurtzite structure. Cadmium sulphide samples prerared from [Cd(thio)2I2] complexes consist of two phase mixture. Together with the main wurtzite modification the phase with zinc blende crystal structure has been observed in these CdS layers. The values of tetrahedral radii of Cl and Br are close to radius of sulfur atom (0,104 nm). During the crystallization process the iodine atoms (r = 0,128 nm) create the essential distortions in crystal structure, which have led to formation of zinc blende phase.

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