The present study aims to investigate the advantages of diamond-like carbon (DLC) films in reducing friction and lubrication to address issues such as the low surface hardness, high friction coefficients, and poor wear resistance of titanium alloys. Cr-doped DLC films were deposited by high-power impulse magnetron sputtering (HiPIMS) in an atmosphere of a gas mixture of Ar and C2H2. The energy of the deposited particles was controlled by adjusting the target powers, and four sets of film samples with different powers (4 kW, 8 kW, 12 kW, and 16 kW) were fabricated. The results showed that with an increase in target power, the Cr content increased from 3.73 at. % to 22.65 at. %; meanwhile, the microstructure of the film evolved from an amorphous feature to a nanocomposite structure, with carbide embedded in an amorphous carbon matrix. The sp2-C bond content was also increased in films, suggesting an intensification of the film’s graphitization. The hardness of films exhibited a trend of initially increasing and then decreasing, reaching the maximum value at 12 kW. The friction coefficient and wear rate of films showed a reverse trend compared to hardness variation, namely initially decreasing and then increasing. The friction coefficient reached a minimum value of 0.14, and the wear rate was 2.50 × 10−7 (mm3)/(N·m), at 8 kW. The abrasive wear was the primary wear mechanism for films deposited at a higher target power. Therefore, by adjusting the target power parameter, it is possible to control the content of the metal and sp2/sp3 bonds in metal-doped DLC films, thereby regulating the mechanical and tribological properties of the films and providing an effective approach for addressing surface issues in titanium alloys.