Tetrahedral amorphous carbon (ta-C) has emerged as an excellent coating material for improving the reliability of application components under high normal loads. Herein, we present the results of our investigations regarding the mechanical and tribological properties of a 2-μm-thick multilayer ta-C coating on high-speed steel substrates. Multilayers composed of alternating soft and hard layers are fabricated using filtered a cathodic vacuum arc with alternating substrate bias voltages (0 and 100 V or 0 and 150 V). The thickness ratio is discovered to be 1:3 for the sp²-rich and sp³-rich layers. The results show that the hardness and elastic modulus of the multilayer ta-C coatings increase with the sp³ content of the hard layer. The hardness reached approximately 37 GPa, whereas an improved toughness and a higher adhesion strength (> 29 N) are obtained. The friction performance (µ = 0.07) of the multilayer coating is similar to that of the single layer ta-C thick coating, but the wear rate (0.13 × 10^-6 mm³/(N·m)) improved under a high load of 30 N. We further demonstrate the importance of the multilayer structure in suppressing crack propagation and increasing the resistance to plastic deformation (H³/E²) ratio.