Nickel-iridium alloys were electrodeposited on copper substrates in a small three-electrode cell, under galvanostatic conditions. The bath solution consisted of iridium (ⅡI) chloride hydrate and nickel sulfamate as the electroactive species, and citric acid as the complexing agent. The effects of bath composition and operating conditions on the Faradaic efficiency (FE), partial current densities, as well as on the thickness of the alloys and their composition were studied. The Faradaic efficiency (FE) and partial deposition current densities were calculated based on mass gain and elemental analysis using energy dispersive spectroscopy. The surface morphology of the alloy was characterized by scanning electron microscopy and atomic force microscopy. The phase and chemical composition the alloys were determined by X-ray diffraction and X-ray photoelectron spectroscopy, respectively. The thickness of the coating was measured on metallographic cross-sections. The results are discussed with emphasis on routes to increase the Faradaic efficiency and iridium content in the alloy. A mechanism for the electrodeposition of nickel-iridium alloys is presented.