Ni/Al alloy powders were synthesized by ball milling of nickel-aluminum powder mixture with a Ni/Al atomic ratio of 1:1. Ni/Al alloy coating was deposited by cold spraying using N2 as accelerating gas. NiAl intermetallic compound was evolved in-situ through post-spray annealing treatment of cold-sprayed Ni/Al alloy coating. The effect of annealing temperature on the phase transformation behavior from Ni/Al mechanical alloy to intermetallics was investigated. The microstructure of the mechanically alloying Ni/Al powder and NiAl coatings was characterized by scanning electron microscopy and X-ray diffraction analysis. The results show that a dense Ni/Al alloy coating can successfully be deposited by cold spraying using the mechanically alloyed powder as feedstock. The as-sprayed alloy coating exhibited a laminated microstructure retained from the mechanically alloying powder. The annealing of the subsequent Ni/Al alloy coating at a temperature higher than 850°C leads to the complete transformation from Ni/Al alloy to NiAl intermetallic compound.