Plasma-polymerized deposition of an acetylene-hydrogen-silane mixture (C2H2-H-2-SiH4) to obtain thin film with good wear behavior on a high-density polyethylene (HDPE) surface was present in this work. It was found that the bond between thin film and HDPE substrate was excellent and H-2 gas in system led the deposited thin film to better adhesive properties, but slower thin film deposition rate. Surface wear-resistant properties of modified HDPE were improved with the input of SiH4. Infrared and X-ray photoelectron spectroscopy spectra suggested that there be large quantities of >C=O, O-H, C-Si, and Si-O groups in thin film and that the ratio of C to Si was increased due to the addition of SiH4 and H-2, which inferred that the thin film structure and components lie between organic and inorganic materials.