In this paper, the wear of nanostructured NiAl coating was studied both experimentally and numerically. First, the nanocrystalline NiAl intermetallic powder was synthesized by mechanical alloying (MA) of aluminum and Ni powders. The coatings were deposited onto the low carbon steel substrate using high velocity oxy-fuel (HVOF) technique. Nanoindentation test was conducted to find out the mechanical properties of the coating. The dry wear tests were then performed using a pin-on-block test rig under different operating conditions. Finally, finite element (FE) method was employed to model the wear characteristics of the prepared nanostructured material. A three-dimensional (3D) FE model was created and used to simulate the pin-on-block experiments. The results show that the volume losses predicted by the numerical analysis are in good agreement with the experimental data.