In the last decade, research has focused on fabricating new materials to accelerate the development of energy storage devices. In this work, metal-electrolyte-metal (Au-YSZ-Ru) structures were fabricated on silicon substrates using atomic layer deposition, sputtering, and thermal evaporation techniques. The effect of the yttrium concentration in YSZ films on their chemical, structural, optical, and electrical properties were studied. XPS analysis showed yttrium concentrations of 14.6, 10.3, 6.8, and 5.3 at.% for films with ALD cycle ratios Zr:Y of 2:1, 4:1, 6:1, and 8:1. Deconvolution of the oxygen XPS signal demonstrate the yttrium to oxygen vacancies ratio. The band gap was calculated through UV-vis indicating an increase in values with yttrium concentration. In addition, the trend was confirmed by reflection electron energy loss spectroscopy (REELS). The structure was investigated by performing X-ray diffraction (XRD) and infrared attenuated total reflectance spectroscopy (IRATR) measurements. Both results indicate a better crystallization of the cubic phase for the samples with lower concentrations, as the intensity of (111) diffraction peaks and IR band increased for lower yttrium concentrations. Impedance spectroscopy revealed an activation energy of 1.69, 1.32, and 1.28 eV for the 10.3, 6.8, and 5.3 at.% film concentration, respectively. According to cyclic voltammetry and charge-discharge tests, a lower yttrium concentration, 5.3 at.%, promotes electrode REDOX reactions improving the energy-storage properties.