Nanocrystalline NiAl intermetallic powder was prepared by mechanical alloying (MA) of Ni50Al50 powder mixture and then deposited on low carbon steel substrates by high velocity oxy fuel (HVOF) thermal spray technique using two sets of spraying parameters. X-ray diffraction (XRD), scanning electron microscopy (SEM), transition electron microscopy (TEM), differential scanning calorimetry (DSC), and hardness test were used to characterize the prepared powders and coatings. The MA of Ni50Al50 powder mixture led to the formation of NiAl intermetallic compound. The resulting powder particles were three dimensional in nature with irregular morphology and a crystallite size of ~10 nm. This powder was thermally sprayed by HVOF technique to produce coating. The deposited coating had a nanocrystalline structure with low oxide and porosity contents. The hardness of coatings was in the range of 5.40-6.08 GPa, which is higher than that obtained for NiAl coating deposited using conventional powders.