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The typical porous structure and the presence of the dangling bonds mainly make the sputtered TMD lubricating film have a short wear life in a vacuum and vulnerable to oxidation or corrosion in moisture, degrading the tribological properties. In this study, periodic N ion bombardment of the deposited MoS2layers was done to obtain a N passivated nanocrystalline MoS2film, and the tribological properties both in a vacuum and in the atmosphere were investigated. It has been demonstrated that by periodic N ion bombardment higher than six times for a MoS2film with a total thickness of about 1.5 μm, the obtained films showed a much lower friction coefficient of 0.020 and a wear life higher than 5.0 × 105sliding cycles in a vacuum compared to about 0.032 and 2.3 × 105sliding cycles for the contrast pure MoS2film. Meanwhile, the periodically N ion dealt MoS2film exhibited a very stable friction coefficient as well as a much longer wear life in a humid environment. The improved tribological properties of the N ion dealt MoS2film were mainly due to the obtained densely distributed MoS2nanocrystals as well as the N passivation of the dangling bonds to inhibit the oxidation of the MoS2in air.