The functional properties of both electrodeposited and sputtered nickel and NiW nanostructured alloys are discussed as a function of their main microstructural features. As W is incorporated into the Ni matrix, several metallurgical parameters that can influence the functional properties were also modified, namely grain size, crystallographic texture, morphology and element contamination. The hardness measurements for the different coatings were analysed in terms of both grain size and W incorporation effects. In addition, the high level of Argon, particularly for the NiW-PVD coating, was shown to be responsible for the highest hardness value obtained. Comparing the behavior of NiW coatings with that of pure nickel in both elaboration processes shows that tungsten incorporation greatly enhances abrasion resistance.