We studied the effect of organic additives on the surface planarity and magnetic properties of electroplated Ni-Fe Permalloy thin films. Compared to thin films prepared with a pure inorganic electrolyte, the Ni-Fe permalloy thin films electroplated with electrolytes containing additives showed changes in their crystalline orientations, surface roughnesses, and coercivities. The reduction in coercivity showed a strong correlation with the observed improvement of the surface planarity. We observed that the surface planarity of the thin films could be improved by 50-60% and that coercivity could be adjusted between 0.33 and 0.05 Oe by changing the concentration of additives.