Abstract: The need for reducing the wear in mechanical parts used in the industry makes self-lubricant films one of the sustainable solutions to achieve long-term protection under different environmental conditions. The purpose of this work is to study the influence of C additions on the tribological behavior of a magnetron-sputtered TiN film in air, water, and seawater. The results show that the addition of C into the TiN binary film induced a new amorphous phase, and the films exhibited a dual phase of fcc (face-centered cubic)-TiN and amorphous carbon. The antifriction and wear-resistance properties were enhanced in air and water by adding 19.1at% C. However, a further increase in the C concentration improved anti-frictional properties but also led to higher wear rates. Although the amorphous phase induced microbatteries and accelerated the corrosion of TiN phases in seawater, the negative abrasion state was detected for all Ti–C–N films due to the adhesion of the tribocorrosion debris on the wear track.