Diamond-like carbon (DLC) film is widely used due to its excellent properties, such as high hardness and high wear resistance. To investigate the advantages of DLC film applied on the surface of Mg alloy, direct current (DC) pulse magnetron sputtering was used to prepare DLC film via plasma sputtering a graphite target and introducing C2H2 gas. The silicon interlayer was fabricated by sputtering the Si target. A scanning electron microscope (SEM), transmission electron microscope (TEM), a nano-indentation instrument, an electrochemical workstation and a pin-on-disc tester were employed to obtain the surface morphology, microstructure, mechanical properties, corrosion behavior and wear resistance of the obtained film, respectively. The results show that the DLC films are dense and compact, and the structure changes from amorphous to nanocrystalline with the increase of C2H2 flow. The film prepared at low C2H2 flow has larger surface roughness, lower deposition rate, higher hardness and elasticity modulus, poorer corrosion resistance and better wear resistance, compared with the film prepared at higher acetylene flow. The self-corrosion potential of the obtained DLC film is higher than −0.95 V, the corrosion current density is 10−7 A/cm2 orders of magnitude, and the wear rate is 10−9 mm3/Nm orders of magnitude. The friction coefficient of the film is less than 0.065, the hardness is 17.3 to 22.1 MPa, and the elastic modulus is 145 to 170 MPa. The DLC films obtained on the surface of AZ91 alloy have good comprehensive properties.