The optimal plating settings in the pulse-reverse electroplating mode for the non-anomalous plating of Fe-Ni deposits (i.e., the metal composition of deposits is equal to that of the plating solutions! from chloride solutions were approached by using experimental strategies including fractional factorial design (FFD), path of steepest ascent, and central composite design (CCD) coupled with response surface methodology. The potentials of pulse plating and reverse plating, pH, and the time period of reverse plating were found to be the key factors affecting the composition of Fe-Ni deposits in the FFD study. The first three variables were subjected to the path of the steepest ascent investigation to approach the optimal conditions for non-anomalous plating of Fe-Ni deposits. The effects of pulse-plating and reverse-plating potentials on the composition of Fe-Ni deposits were further examined using a regression model in the CCD study. This model, represented as response surface contour plots, showed that the composition of an Fe-Ni deposit plated from the bath with pH of 2.8, a pulse-plating potential of -1290 mV, reverse-plating potential of -84 mV, pulse-plating time of 360 ms, and a reverse-plating time of 120 ms was equal to the composition of metal ions in the plating bath. Based on these optimal plating settings, the composition of Fe-Ni alloys can be precisely controlled by adjusting the composition of the plating baths.