Chlorine implantation into TiN coatings decreases the wear loss and the friction coefficient. Even by low-dose chlorine implantation, the wear volume is decreased by three orders of magnitude or more, and the friction coefficient becomes <0.1. This self-lubrication mechanism is related to the presence and mobility of implanted chlorine atoms inside the columnar TiN microstructure. According to observations of chlorine-implanted TiN coatings using high-resolution transmission electron microscopy, the chlorine atoms are present in the damaged region, where TiN is composed of nanosized grains. From these data, a self-lubrication mechanism is proposed with chlorine catalyzing the oxidation of titanium and leading to the formation of some tribological reaction product.