Tetrahedral amorphous carbon (ta-C) films with bias-regulated (namely from −50 V to −200 V) Ti interlayers were prepared on AISI 440C stainless steel substrates, followed by systematic investigation on the microstructure, mechanical, and adhesion properties of such films. In addition, molecular dynamics simulation has been employed to study the formation of Ti films deposited with different incident energy, which was found to be influenced by the bias voltage significantly. The experimental results demonstrated that varying bias voltage on the Ti interlayer exerted minor influence on the sp 3 C fraction and mechanical properties of ta-C films. Molecular dynamics simulations showed further support for the experimental results. The Ti interlayer exhibited the amorphous-like microstructure, and increasing Ti-atom incident energy resulted in increasing Ti/Fe interlayer thickness and a firstly rising and then descending Fe/Ti interfacial bonding strength. The adhesive failure mode can be divided into buckling crack and interfacial spallation, which was primarily attributed to the tensile-to-compressive transformation of the Ti-interlayer internal stress. Optimised adhesion property of ta-C films can be achieved with a Ti-interlayer bias voltage of ∼ -100 V. • The effects of interlayer bias voltage on the mechanical properties was studied. • The highest adhesion strength was obtained with voltage bias of −100 V in the Ti interlayer. • MD simulations to clarify the relationship between the adhesion and the Ti ions incident energy.