In the OLED display manufacturing process, a fine metal mask (FMM) is used for the RGB side-by-side in precise positions. An Invar alloy with exceptionally low thermal expansion was used as the FMM material to prevent the deformation of the FMM by heat during the deposition process. The thickness of the FMM must be reduced to less than 10 microns to manufacture high-resolution OLED displays, making it essential to apply a bottom-up electrodeposition process. Moreover, controlling the interfacial energy of the cathode substrate and the electrolyte is necessary to achieve ion electrodeposition and peeling of the ultra-thin Fe-Ni plated on the cathode substrate during electrodeposition. Therefore, this study investigated the effect on the properties of the electrodeposited Fe-Ni alloy by controlling the amount of SLS content, which acts as a surfactant. The amount of SLS content was maintained in the range of 0 to 1 g/L, and the composition homogeneity, microstructure, and surface defects of the electrodeposited Fe-Ni alloy were investigated. Under low pH conditions, the composition was insignificantly changed depending on the difference in the amount of SLS content, and a uniform composition was observed. The findings of this research offer valuable insights for optimizing the electrodeposition process, which is crucial for producing high-resolution OLED displays with ultra-thin FMM, advancing display technology.