Diamond-like carbon (DLC) films with high sp3 C–C bonding percentage are currently referred to as ta-C (tetrahedral amorphous carbon) [1]. Due to the special excellent properties such as extreme hardness, better mechanical properties, low friction, optical properties, electric properties, thermal stability properties and thermal conductance properties, ta-C has been widely concerned [2]. Filtered cathodic vacuum arc deposition (FCVA) is main method to deposit ta-C [3], because the FCVA technique can separate the carbon plasma from the macroparticles by magnetic–electric filters and deposit films with more smooth surfaces than traditional vacuum arc deposition methods. In order to improve the deposition efficiency of ta-C and realize large-scale industrial application of ta-C, a rectangular filtered cathodic vacuum arc deposition has been developed [4] and used to deposit ta-C in this study. To release the high-level internal stress due to the mismatch of high sp3 content, the W layer was deposited alternatively after the deposition of ta-C film and thus alternative ta-C/W multilayer films were obtained. Variations modulation ratios (thickness ratio of the W layer to ta-C layer) ranging from 2:1, 1:1 to 1:2 were studied to get the optimal modulation ratio. According to optimal the modulation ratio, variations modulation periods ranging from 300nm, 450nm to 600nm were studied. Before the deposition, a 300 nm thick Cr layer and a 700 nm thick W were deposited as the intermediate layer. The relationship between the film mechanical properties, such as hardness, adhesion strength, and their microstructure was researched. The detailed bonding structure of DLC film was obtained by Raman spectroscopy. Morphology and thickness of multilayered film were measured by examining fractured cross-sections using scanning electron microscopy. The hardness of multilayered film was obtained by nanoindentation. The adhesion strength was evaluated qualitatively by Rockwell indentation test.