The research clarified the relationship between applied deposition bias voltage and the resulting bonding structure evolution, which directly adjusts corrosion resistance and tribological properties of multilayered tantalum-containing carbon coatings. Comparative analysis of bonding structure revealed that the preferential orientation of the tantalum carbide structure shifts from TaC (200) to TaC (111) as the bias voltage ranges from -75 V to -125 V. The TaC (111) structure significantly enhances chemical stability and anti-deformation ability, contributing to low corrosion current and specific wear rate. The graphite structure formed in the coating deposited at a bias voltage of -175 V effectively contributed to the lowest friction coefficient. However, the friction advantage is accompanied by decreased mechanical strength and accelerated wear.