The nano-indentation response and the friction/wear properties of DLC/SiC (diamond-like carbon/silicon carbon) double layer thin films deposited on Mg alloy (AZ91D) substrate using magnetron sputtering technique at room temperature were investigated. The results show that the DLC films displayed low nano-hardness (3.05 GPa), low Young's modulus (24.67 GPa) but high hardness-to-modulus ratio (0.124). The films-substrate system exhibited a good friction and wear properties with the mean friction coefficient of about 0.175, the special wear rate in the magnitude order of 10−6 mm3 m−1 N−1 together with little film-cracking and interface-delaminating, when sliding against Si3N4 (silicon nitride) ball using ball-on-disc wear tester under dry frictional condition. The high wear-resistance is in accordance with high ductility of the films, good modulus match in the films-substrate system, and high hardness-to-modulus ratio of the films. The underlying factors are discussed and are believed to be due to the substrate is Mg, a metal with high activity.