Aspects of the present disclosure are directed to electrochemical approaches for synthesis of platinum-iridium alloys with selected platinum-iridium ratio content and subsequently predetermined mechanical properties and electrochemical impedance properties. Such can provide a simple and cost-effective process for preparing these electrodes, as compared to conventional thin film processing techniques. A three-electrode electrochemical electrodeposition system is described including an electrochemical cell with a working electrode on which the electrodeposited film is deposited, a counter electrode to complete the electrochemical circuit and a reference electrode to measure and control surface potential. Mixed layers of platinum atoms and iridium atoms can be deposited from electrolyte solution onto the working electrode surface to create an electrically conductive surface with material properties related to the composition of the as-deposited film. The mechanical properties and electrochemical properties of the film can be tuned by adjusting the electrodeposition parameters.