The aim of this work is to study the effect of surface treatment of a polypropylene film with low-pressure plasma using CH4-O-2 mixture gas in an 80:20 ratio. The effect of the variation of the plasma treatment conditions has been studied to optimize the plasma effects. The film wettability has been analyzed by the study of the variation of free surface energy and its polar and dispersive components. The surface functionalization of the PP film was also analyzed by X-ray photoelectron spectroscopy (XPS) and attenuated total reflectance infrared spectroscopy (FTIR-ATR) analysis. The surface topography was analyzed by scanning electron microscopy (SEM) and atomic force microscopy (AFM). The CH4-O-2 plasma treatment induces the ablation inherent of a traditional plasma treatment and polymerization mechanisms to take place simultaneously at the treated surface. The PP film treated with CH4-O-2 plasma shows a remarkable improvement on the surface free energy mainly caused by surface functionalization as XPS reveals. Slight changes in surface topography are observed, but they do not contribute in a significant way to improve wettability.