Poor surface finish and coarse dendrite structure are the major challenges in direct-current ͑dc͒ plating of nanosized Ni-Cu alloy coatings. This investigation was initiated to understand the effect of saccharin on the formation of nanosized Ni-Cu alloy coatings by sediment codeposition, and the role of saccharin in improving surface finish and suppressing coarse dendrite growth during sediment codeposition. It was found that only 0.5 g/L addition of saccharin could form dendrite-free nanocrystalline Ni-Cu alloy coatings with a mirror-finish surface. The Cu content in the Ni-Cu alloy coatings can be controlled to be as low as 10 wt % by changing the current density. The grain size in the coatings was determined by X-ray diffraction and electron microscopy analysis to be 15.7 nm on average. The amount of ordered L1 0 -type Ni-Cu nanophase was found to be insignificant in comparison with that in pulse plated coatings. Saccharin suppresses the reduction of Cu and acts as a leveling and grain size reduction agent in Ni-Cu alloy codeposition. From steady-state polarization and impedance analysis, it is believed that these saccharin effects are produced by the formation of Ni-Saccharin complexes adsorbed on the coating surface that suppress Ni-Cu dendrite growth.The electrodeposition of nanostructured materials has attracted considerable interest in the past several decades because of its distinct advantages in preparing thin-film materials. 1 Low fabrication temperatures minimize interdiffusion during deposition. Uniform films with controllable thicknesses and compositions as well as a pore-free structure can be easily obtained. Moreover, electrodeposition is cost-effective. The electrodeposited nanomaterials demonstrate many advanced properties and have been utilized as tribological materials, corrosion resistant materials, magnetic materials, and noble metal catalysts. [2][3][4][5][6] Among these, electrodeposited nanocrystalline ͑nc͒-Ni-Cu alloys and their multilayers 3 have received growing attention because of their improved resistance to pitting corrosion 3 and giant magnetoresistance properties. 7 The dc plating of Ni-Cu alloy coatings is normally performed above a critical current density to form a thick and crack-free layer of deposits of known composition. A continuous current flow through the solution in dc plating promotes dendrite growth and the formation of a rough surface. 8 The deposition of nanosized Cu-Ni alloy coatings through dc plating requires the application of much higher current densities, which would further deteriorate the surface finish of the coatings, and can result in the formation of cracks and pores in the deposits. 9 Ghosh et al. 10 reported that powdery deposits could form at current densities of 30-40 mA/cm 2 in dc plating. Many efforts have been made to avoid this problem, for example, by pulse current ͑PC͒-plating ncNi-Cu multilayers. 3,10,11 So far, however, no research has been reported to prepare dc-plated nanosized Ni-Cu alloy coatings with a surface finish comparable to that ...