Surface fluorination with pure F2 gas can easily make the surface on PP (polypropylene) hydrophobic, and it causes limited dyeability, as reported in a previous paper. In this study, to produce a more hydrophilic surface, surface fluorination of PP was performed at 25 °C, total gas pressure of 13.3 kPa, and reaction time of 1 h using F2 and O2 mixtures with different proportions of F2 gas. The surface roughness of the fluorinated PP samples was about 1.5 times higher than that of the untreated sample (5 nm). Fourier-transform infrared spectroscopy and X-ray photoelectron spectroscopy (XPS) results showed that the PP-derived bonds (-C-C- and -CHx) decreased because they were converted into polar groups (-C–O, -CHF-, and -CFx), which increased the surface electronegativity of the PP. The variation in the F2 gas proportion in the gas mixture significantly affected the hydrophilicity and surface composition of the PP. At F2 gas proportions of <70%, the hydrophilicity of the fluorinated PP samples was increased. Notably, the hydrophilic and negatively charged PP surface enhanced the dyeing of the polymer with basic methylene blue (MB). In contrast, at F2 gas proportions of >90%, the PP surface became hydrophobic owing to increased numbers of hydrophobic -CF3 bonds. Thus, enhanced PP dyeing can be controlled based on the composition of the F2 and O2 gas mixture.