Aniline and phenylacetylene and their derivatives are important compounds in chemical industries [1]. Diazonium salts are highly useful intermediates in the synthesis of a large variety of aromatic compounds. These can be used to prepare many classes of organic compounds. Aryl diazo compounds are brightly colored and are useful as dyes and pigments so are classified as azo dyes. Azo compounds are good oxidizing agents and can be readily reduced back to hydrazine or a primary amine. Additionally, azo compounds have been utilized in various biological assays, as coupling agents, and in synthetic dyes [2]. Diazo compounds exhibit high synthetic versatility, spanning organic and inorganic chemistry. Diazo compounds can be used to couple and immobilize biomolecules onto surfaces [3]. In this work we study the electrochemical oxidation of 4-ethynylaniline, using coloumetery at controlled potential technique at the surface of the graphite electrode as a working electrode at various pH. The results revealed that the diazo compound was synthesis by 4-ethynylanilin at the specific pH in the divided cell using coloumetery at controlled potentials. The purity of product and characterization was done using 1H NMR, 13C NMR, FTIRspectroscopic techniques. The presented strategies use a water/acetonitrile mixture as solvent. These strategies represent a one-pot and facile process for the synthesis of diazo compound in high yield and purity.