In recent years, nickel-cobalt alloys are considered as high temperature and microwave applications due to high magnetic transition temperature and absorbing properties of waves. This alloys also are used in the electronics industry for the manufacture of magnetic memory in devices of computers. Watts type solution is the most common solution of cobalt- nickel alloy electro depoition. In the present research, for evaluate the effect of anions in Watts solution, the effect of chloride and sulfate ions on the nickel-cobalt alloy was studied and the results showed that an increase in chloride ion respect to sulfate ion, reduced the amount of cobalt at high current density (90 mA / cm 2 ) and increased the percentage of cobalt in low current density (10 mA / cm 2 ). In order to optimize Watts electrolytes and to remain constant the ionic strength parameters in the bath of a different composition, the total concentration of anions and cations were considered constant. By producing different combinations of alloys, was observed that increasing cobalt percentage in coating cause to change structure from fcc to hcp +fcc and then hcp phase decreases with more increasing cobalt content. Using salt bridge in nickel-cobalt bath resulted in reduce anomalous deposits of cobalt in high current density. In order to improve the properties of nickel-cobalt alloy, carbon nanotubes were added to the alloys. The results showed that cobalt-nickel /carbon nanotubes nanocomposite with high cobalt percentage had a higher saturation magnetization and less coercivity compared to alloy sample and even to pure cobalt. In this study a new electrodeposition bath also introduced that named as lithiumic bath of nickel-cobalt electrodeposeton. This bath that was gained by replacing some percent of cobalt and nickel sulfate with lithium sulfate cause to decrease anomalous deposite of cobalt, increase the percentage of carbon nanotubes in the composite coating, increase the grain size and the prefrential growth direction respect to Watts solution. The price of this bath is much lower than Watts ones. Keywords : Nanocrystalline materials, Nickel-cobalt alloy, Carbon nanotubes, Magnetic properties, Anomalous deposition, Cobalt-nickel