In this thesis, two derivatives of pheylcyanamide ligands, including 4-Cl, 4-NO 2 pheylcyanamide have been synthesized and characterized by FT-IR and UV-Vis spectroscopies. By using these ligands and hexamethylenetetramine ligand, complexes of Cu (II) and Co (II) have been synthesized. These complexes have been characterized by FT-IR, UV-Vis and were investigated by fluorescence spectroscopy, cyclic voltammetery and paramagnetic 1 H-NMR. FT-IR spectrum of theses complexes show that vibrational modes of C?N band have been shifted to higher frequencies in comparsion to free substituted heylcyanamide ligands. Also, vibrational mode of C-N band in hexamethylenetetramine, in these two complexe has been shifted to higher frequencies, which proved the linkage of this ligand to each central metal. Electronic spectrum of these two complexes was taken in DMF and acetonitrile solutions. The keen absorption bonds in UV region are assigned to ligands-centered transitions and weak absorption in visible region are assigned to d-d transitions in metal center. Fluorescence spectrum of these two complexes , was taken in DMSO solution. Emission spectrum of these two complexes shows linkage pheylcyanamide ligand to central metal. Cyclic voltamogram of two complexes was recorded in DMF solution with TBAH as supporting electrolyte and at room temperature. Paramagnetic 1 H-NMR spectrum of two complexes was recorded in the deoxygenation DMSO-d 6 . In comparsion of synthesized complexes, there are greater variety of signals for Cu(II) complex due to dimeric structure of it. Finally, calculations of the magnetic susceptibility for the two complexes was done based on Evans method..