A novel surface modification method was proposed to improve the tribological property of Si. Multilayers were grown on Si(100) substrate by self-assembling monolayer (SAMs) method and filtered catholic vacuum arc (FCVA) technique. The film composition and structure were characterized by using x-ray photoelectron spectroscope (XPS) and Raman spectroscopy (Raman). Surface morphology and the roughness were also analyzed by an atomic force microscope (AFM) and a scanning electron microscopy (SEM). The frictional behaviors of the films were evaluated by a UMT tester. Results showed that elastomeric nanocomposite monolayer prepared by SAM was uniformly distributed and isotropy, and the diamond-like carbon (DLC) film was successfully deposited by the FCVA technique. The friction coefficients of the prepared samples were in the range of 0.108-0.188. Furthermore, the friction coefficient slightly increased but the surface quality of the wear trace was improved after adding the copolymer elastomeric macromolecules SEBS on aminopropyl-triethoxysilane (APS) layer due to the inherent long chain of SEBS which abated the immediate impulsion at the interface and changed the kinetic energy into elastic potential energy, and stored it in SEBS. A novel surface modification method was proposed to improve the tribological property of Si. Multilayers were grown on Si (100) substrate by self-assembling monolayer (SAMs) method and filtered catholic vacuum arc (FCVA) technique. by using x-ray photoelectron spectroscope (XPS) and Raman spectroscopy (Raman). Surface morphology and the roughness were also analyzed by atomic force microscope (AFM) and a scanning electron microscopy (SEM). The frictional behaviors of the films were evaluated by a UMT tester. Results showed that elastomeric nanocomposite monolayer prepared by SAM was uniformly distributed and isotropy, and the diamond-like carbon (DLC) film was successfully deposited by the FCVA technique. The friction coefficients of the prepared samples were in the range of 0.108-0.188. In addition, the friction coefficient slightly increased but the surface quality of the wear trace was improved after adding the copolymer elastom eric macromolecules SEBS on aminopropyl-triethoxysilane (APS) layer due to the inherent long chain of SEBS which abated the immediate impulsion at the interface and changed the kinetic energy into elastic potential energy, and stored it in SEBS.