A stable and improved control of the wettability of textiles was obtained by using a coating of diamond like carbon (DLC) films on cotton by PECVD. By controlling different plasma pretreatments of argon, oxygen, and hydrogen on the cotton fibers' surface, we have shown that the pretreatments had a significant impact on wettability behavior resulting from an induced nanoscale roughness combined with an incorporation of selected functional groups. Upon subsequent deposition of diamond like carbon (DLC) films, the cotton fibers yield to a highly controlled chemical stability and hydrophobic state and could be used for self-cleaning applications. By controlling the nature of the plasma pretreatment we have shown that the oxygen plasma pretreatment was more effective than the argon and hydrogen for the superhydrophilic/ultra hydrophobic properties. The chemical and morphological changes of the cotton fibers under different treatments were characterized using X-ray photoelectron and Raman spectroscopy, AFM, and water contact angle measurements. The mechanism underlying the water-repellent properties of the cotton fibers provides a new and innovative pathway into the development of a range of advanced self-cleaning textiles.