We investigated the effects of organic additives on the properties of nickel-copper thin films prepared by electroplating. Compared with thin films fabricated by pure electrolyte only, the films utilizing organic additives show different crystalline orientations. With no alteration of plating conditions simply adding the organic materials changed the composition of copper and nickel. The concentration of nickel could be varied to $65-95\%$ depending on the species and concentration of the additives. The change of material property has contributed to the increase or decrease of the magnetoresistance.