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A series of (AlCrTiZrV)-Six-N films with different silicon contents were deposited on monocrystalline silicon substrates by direct-current (DC) magnetron sputtering. The films were characterized by the X-ray diffractometry (XRD), scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), and nano-indentation techniques. The effects of the silicon content on the microstructures and mechanical properties of the films were investigated. The experimental results show that the (AlCrTiZrV)N films grow in columnar grains and present a (200) preferential growth orientation. The addition of the silicon element leads to the disappearance of the (200) peak, and the grain refinement of the (AlCrTiZrV)-Six-N films. Meanwhile, the reticular amorphous phase is formed, thus developing the nanocomposite structure with the nanocrystalline structures encapsulated by the amorphous phase. With the increase of the silicon content, the mechanical properties first increase and then decrease. The maximal hardness and modulus of the film reach 34.3 GPa and 301.5 GPa, respectively, with the silicon content (x) of 8% (volume percent). The strengthening effect of the (AlCrTiZrV)-Six-N film can be mainly attributed to the formation of the nanocomposite structure.