The coordination chemistry of Phenylcyanamide and its substituted derivatives began with a study by Hollebone in 1971 but remined largely unexplored until the late 1980s. This is surprising as the coordination chemistry of Phenylcyanamides should-be as rich as that of other Pseudohalides such as azide and thiocyanate. Indeed, the attachment of a Phenyl ring to the cyanamide group adds an extra dimension not present in azide or thiocyanate ligands. An extensive ? conjugation between the cyanamide group and the phenyl ring provides an energetically favorable means by which a metal ion can couple into a conjugated organic ? system. The Phenylcyanamides are ambidentate ligands whether neutral or in anionic form and so the possibility of linkage isomerism must be recognized. Phenylcyanamide and its derivatives can be readily prepared in high yields from the corresponding anilines by desulfurization of the thiourea derivative. In this project, first the ligands of 4-NO 2 Pcyd, 4-FPcyd, 4-ClPcyd, 4-BrPcyd and then Silver(I) complex with the ligand of 4-NO 2 Pcyd and Mercury(II) complexes with these four ligands were synthesized and characterized by IR, UV-Vis spectroscopy techniques. Neutral Phenylcyanamides can coordinate to a metal ion through either the nitrile or amine nitrogen. However, at this point in time, there are no crystal structures of neutral Phenylcyanamides coordinated to metal ions. The amine nitrogen is sterically crowded by the phenyl ring and so terminal coordination to the cyano nitrogen is expected, particularly for electron-rich metal centers. Metal ions that behave as ?-donor properties. Side-on coordination of the cyanamide group has not been observed for Phenylcyanamide ligands but has been observed in tungsten complexes of dialkylcyanamides. There are many crystal structures of monodentate Phenylcyanamide ligands showing coordination through the cyano nitrogen but there are no examples of amine-nitrogen coordination. Both neutral or anionic Phenylcyanamides can function as bridging ligands although this has only been observed for the anionic cyanamides but for the first time in this project in [Hg(4-NO 2 Pcyd)(CH 2 OCH 3 )] n complex that molecular structure was determined by X-Ray crystahhography, coordination of 4-NO 2 Pcyd ligand to Hg(II) unexpectedly occurred through amine-nitrogen, that this point is very notable. Another interesting phenomenon in this project is formation an Organometallic compound that have been produce by linkage of oxygen atom of acetone to Hg(II) that it’s very important. At the next part of this project, Electrochemical manner of complex [Ag(4-NO 2 Pcyd)] n investigated as Modified Electrode in measurement Dibucaine drug. Dibucaine is an amide local anesthetic.