This study was designed to examine the photoelectric device performances of cobalt-iron (CoFe) and cobalt-iron-nickel (CoFeNi) materials with good magnetic properties, specifically to investigate the effect of the Ni element on theelectrical properties. In this context, Al/CoFe/p-Si and Al/CoFeNi/p Si devices were produced by coating both materia- ls between the semiconductor and the metal using the RF sputtering method. First of all, to investigate the structural properties of the coated films, the content analysis was carried out by X-ray diffraction (XRD) analysis. To determine the photoelectrical properties of the produced devices, current-voltage and transient photocurrent measurements were performed and analyzed under different light intensities. It was determined that both devices are sensitive to light, with the sensitivity of the device with the CoFeNi interlayer being much higher. In addition, photocapacitance and photoconductivity measurements were carried out to examine the photocapacitor performance of the devices. As a result of the investigations, both current-voltage, photocurrent, and photo-capacitance/conductivity measurements showed that the device with the CoFeNi interface layer showed better performance than the device with the CoFe interface. Therefore, it has been determined that the Ni element has a positive effect on electrical properties. Additionally, the results obtained show that the prepared materials and produced devices can be used in photovoltaic applications.