In this work, diamond-like carbon (DLC) films were deposited on stainless steel substrates with Si/SiC intermediate layers by combining plasma enhanced sputtering physical vapour deposition (PEUMS-PVD) and microwave electron cyclotron resonance plasma enhanced chemical vapour deposition (MW-ECRPECVD) techniques. The influence of substrate negative self-bias voltage and Si target power on the structure and nano-mechanical behaviour of the DLC films were investigated by Raman spectroscopy, nano-indentation, and the film structural morphology by atomic force microscopy (AFM). With the increase of deposition bias voltage, the G band shifted to higher wave-number and the integrated intensity ratio ID/IG increased. We considered these as evidences for the development of graphitization in the films. As the substrate negative self-bias voltage increased, particle bombardment function was enhanced and thesp3-bond carbon density reducing, resulted in the peak values of hardness (H) and elastic modulus (E). Silicon addition promoted the formation of sp3 bonding and reduced the hardness. The incorporated Si atoms substituted sp2- bond carbon atoms in ring structures, which promoted the formation of sp3-bond. The structural transition from C-C to C-Si bonds resulted in relaxation of the residual stress which led to the decrease of inteal stress and hardness. The results of AFM indicated that the films was dense and homogeneous, the roughness of the films was decreased due to the increase of substrate negative self-bias voltage and the Si target power.