ZrO2/Ni nanocomposite was produced via pulse electrodeposition using a nickel sulfmate bath. The effects of main factors including pH value, temperature T, current density Dk and ZrO2 content p on the electrodeposit were dealt with by the Taguchi method. Experimental results show that the current density and ZrO2 content affect the electrodepositing process significantly. Nanocomposite with an average grain size of about 50 nm and ZrO2 content of up to 0.4 wt% was produced under the optimal condition. The Young’s modulus of the achieved composite is similar to that of polycrystalline Ni. The microhardness is much higher than that of common pure Ni, primarily due to the ultrafine grains of Ni matrix by the Hall-Petch mechanism. The homogeneous dispersion of stiff ZrO2 particles in the Ni matrix acting as dislocation pinning and microcrack pinning also results in the strengthening effect.