Incorporation of fluorinated multiwalled carbon nanotubes (MWCNTs) into poly(dimethylsiloxane) (PDMS) was studied as an alternative method to improve the surface properties of the latter. The surface properties of PDMS matrixes filled with fluorinated MWCNTs were investigated and compared to those of pristine MWCNT/PDMS composites. Contact angle measurements and attenuated total reflectance infrared spectroscopy revealed that the surface segregation of the fluorinated MWCNTs in PDMS led to changes in the surface chemical composition. The wetting behavior of PDMS when loaded with fluorinated MWCNTs changed relative to that of unfilled samples and samples filled with pristine MWCNTs. Atomic force microscopy showed that the surface roughness of the PDMS increased in the presence of both pristine and fluorinated MWCNTs. Determination of the surface stability of the samples in water demonstrated that fluorinated MWCNTs are more effective than pristine MWCNTs in stabilizing PDMS.