Ti6Al4V alloy is promising biology material with outstanding properties of low density, high specific strength, and exceptional corrosion resistance. However, one of its disadvantages is the poor tribological property. In this paper Mo-N hard surface modification layers were formed on Ti6Al4V at 900°C substrate temperature by plasma reactive sputtering. The flux ratio N2/Ar is an important parameter and its influence on the composition, structure and hardness of the Mo-N layers is studied. The Mo-N layers are duplex layers, composed of diffusing layer and surface coating. The component of Mo and N elements in the diffusing layer changes gradually which can enhance the load-bearing capacity to the coating and ensure the durability of the coating. With the increase of the flux ratio N2/Ar, the content of N element in the Mo-N layers increases. The Mo-N layers were polycrystalline γ- Mo2N with (200) plane oriented parallel to the substrate surface. The surface hardness of the formed layers is in the range HK1330-1430. The hardness of the Mo-N layers increases with the increase of the flux ratio N2/Ar and the reason is that the content of N element in the Mo-N layers increases.