Magnetic alloys are a type of engineering materials which are widely used in various industries such as computers, aerospace and electronics. Among these alloys, Ni-Co alloys were of particular interest. In this study Ni-Co nanocrystalline alloys were prepared by electrochemical deposition method (direct and pulse current) and the effect of current density and electrolyte pH when direct or pulse current were used, on the properties of the obtained deposition was investigated. The result of EDS tests have shown that by increasing current density from 70 to 115 mA/cm 2 , the Cobalt content in deposited alloys is decreased from 70 to 48 wt% in pH=4 and 70 to 50 wt% in pH=1.5, but always the ratio of Cobalt to Nickel in the alloy is higher than that in the electrolyte. This is due to the anomalous simultaneous deposition of Ni-Co. In constant current density by decreasing pH from 4 to 2, the Co content of the alloy is decreased from 70 to 42 wt%, however, by further decreasing of pH to 1.5, a 70 wt% increase in Co content was observed. By applying pulse current and by changing the “pulse off ” time from 50 to 150 µs, Co in alloys was increased from 69 wt% to 76 wt%, and with further increase in the “pulse off” time, Co content fell sharply to 41 wt%. The X-ray patterns, indicated that Ni-Co alloys are solid solution in the whole range of their composition. By controlling of the pH and current mode (direct or pulse), single-phase structure (fcc) and two-phase structures (fcc +hcp) can be obtained. So that, in pH=1.5 at direct current or in pH=1.5, 4 at pulse current process just single-phase structure (fcc) was obtained. The grain size of deposited alloys in direct and pulse current were 24-58 and 15-24 nm, respectively. Studies on the magnetic properties of prepared alloys using AGFM analysis have shown that by increasing the Cobalt content in the alloy and also creating single-phase structure (fcc), magnetic saturation is increased. However, the coercivity of the synthesized alloys was determined at about 40Oe. So the synthesized alloys can be categorized as soft magnetic materials. Keywords: Electrochemical deposition; Nickel-Cobalt alloys; Nanostructures; Soft magnetic materials.