Effects of the pulse bias frequency on the microstructure and properties of TiSiN/TiAlN nano-multilayer films were investigated for optimizing the process parameters and improving the performances. The TiSiN/TiAlN nano-multilayer film were deposited by arc ion plating technology with defferent pulse bias frequency on M2 high-speed steel and monocrystalline silicon substrates. The surface morphology, element composition, cross-section morphology, phase structure and nanohardness of the TiSiN/TiAlN nano-multilayer films were investigate by scanning electron microscope (SEM), energy spectrometer (EDS), X-ray diffractometer and nanoindenter. The diameter of the macroparticles on the surface of the TiSiN/TiAlN nano-multilayer film was mainly concentrated below 1 μm. With the change of the pulse bias frequency, the number of macroparticles was 184~234, and the area was 40.686~63.87 μm2. The main elements of TiSiN/TiAlN nano-multilayer films were Ti and N, which reached to 48% and 50%, respectively. The contents of Si and Al were small. The multilayer structure was not obvious from the cross-sectional morphology, and columnar crystals of TiSiN/TiAlN nano-multilayer films refined. Flaky structure of the crystals appeared at 80 kHz. The TiSiN/TiAlN nano-multilayer films were crystallized with preferred orientation (111) crystallographic planes. The grain size was about 20 nm. The nano hardness was between 28.3~32.3 GPa, and the elastic modulus was between 262.5~286.8 GPa. The number of macroparticles on the surface of the TiSiN/TiAlN nano-multilayer films reached the minimium 184 at 50 kHz. The area occupied by macroparticles reached the minimium 40.686 μm2 at 70 kHz. the grain size was refined at 50~60 kHz. The grain size reached the minimum value of 19.366 nm at 60 kHz. The nano-hardness and the elastic modulus reached the maximum values of 32.3 GPa and 308.6 GPa, respectively. 50~70 kHz was the best the pulse bias frequency range.