Electrodeposition of nanostructured titanium-nickel films was performed and the effect of the concentration of the titanium source on the film characteristics was investigated. Scanning electron microscopy indicated circular crystallites on the surface of the electrodeposited titanium-nickel film with a fairly uniform size distribution. XRD studies showed that the electrodeposited TiNi films contained TiNi with a preferred crystallographic orientation of [002]. Surface analysis using X-ray photoelectron spectroscopy (XPS) revealed that the electrodeposited titanium-nickel film contained elemental titanium and nickel, hydroxide of nickel, and oxides of titanium and nickel. As the titanium ion concentration was increased, the titanium content in the film was increased while the deposition rate and crystallite size of the film were decreased. A blue-shift in the UV/Vis peak was also observed with increasing titanium ion concentration.