In this thesis four derivatives of phenylcyanamide ligands, including 4-F, 4-Cl, 4-Br and 4-NO2phenylcyanamide have been synthesized and characterized by FT-IR and UV-Vis spectroscopies. By using these ligands and 4-aminopyridine as an auxiliary ligand, polymeric complexes of Cu(II) and Ni(II) have been synthesized. These complexes have been characterized by FT-IR and UV-Vis spectroscopies. FT-IR spectrums of these eight complexes show that vibrational modes of C?N band have been shifted to higher frequencies in comparison to free substituted phenylcyanamide ligands. Also the vibrational mode of pyridine ring i 4-aminopyridine, in each of these eight complexes has been shifted to higher frequencies, which proved the linkage of this ligand to each central metal. Electronic spectrum of these eight complexes was taken in DMF solution. The keen absorption bonds in UV region are assigned to ligand-centered transitions and weak absorptions in visible region are assigned to d-d transitions in metal center. For complexes that contain 4-NO2pcyd strong bond in 450nm is assigned to this ligand which is highly colored. More, for producing new cyanamide derivatives, we decided to work on pyridine-cyanamide ligands by using 4-Aminopyridine as raw material, the procedure was the same as which have been used for phenylcyanamide derivatives with slight changes. Finally the thiocyanate salt of 4-aminopyridine have been prepared and characterized with FT-IR spectroscopy. Solid state structure of this salt was determined by single crystal X-ray diffraction crystallography. White crystals of [(4-apyH)+(SCN)-] were grown by slow evaporation of an Acetone/CH2Cl2 solution of this salt. Pyridil nitrogen atom is protonated and SCN- anion is stand in 3.328? across to N+. For preparing hetero nuclear dimer complex of Cu(II) / Ni(II); in first step by using the anionic forms of 4-Chlorophenylcyanamide, 4-Nitrophenylcyanamide and 2,2’-bipyridine ligands, four complexes with general formula [NiCl(Xpcyd)(bpy)2] and [CuCl(Xpcyd)(bpy)] have been prepared and characterized by FT-IR and UV-Vis spectroscopies. Solid state structure of [NiCl(4-NO2pcyd)(bpy)2] has been determined by single crystal X-ray diffraction crystallography. Brown crystals of this complex were grown by ether diffusion into Acetonitrile solution of the complex. In this complex Ni(II) is six coordinated and the bipyridine ligands are coordinated as bidentate ligands. The phenylcyanamide ligand is coordinated from nitrogen atom of nitril group. FT-IR spectrum of all these four complexes show shifts in vibrational modes of C?N bonds to higher frequencies in comparison to free phenylcyanamide ligands. Electronic spectrums of these complexes were taken in Acetone. The intense absorption bonds in the UV region are assigned to ligand centered transitions and a weak absorption bonds in visible region refers to d-d transitions in metal centers. Then by usage of [CuCl(4-Clpcyd)(bpy)] and [NiCl(4-Clpcyd)(bpy)2] in the presence of pyrazine as bridge ligand, the hetero nuclear dimer has been synthesized and characterized by FT-IR and UV-Vis spectroscopies, which have been shown changes in comparison to free ligands and monomer complexes. In FT-IR spectrum of this complex shift of nitril group’s vibrational mode can clearly be seen in comparison with free ligand. UV-Vis spectrum of this complex was taken in acetone solution which shows the intense absorption in UV region that assigned to ligand centered transition, also d-d transitions and charge transfer transitions are clearly objective in this complex.