In order to successfully prepare a new advanced TiAlSiN gradient coating with Ti content gradually decreased but Al content gradually increased from the cemented carbide substrate to the outermost coating surface by arc ion plating, we deeply investigated the influence mechanisms of two important process parameters. These parameters include substrate bias voltage and arc current, which affect the mechanical properties and microstructure of the gradient coating. The results show that bias voltage and arc current directly affect the particle accumulation effect on the coating surface and the re-sputtering effect caused by high-energy ion bombardment, thus affecting the deposition efficiency of the coating and the formation of defects such as macro-particles and pits on the coating surface. The increase of bias voltage is conducive to the increase of the density of columnar crystals and nanocrystals. While the increase of arc current makes the coating with high Al content transform from columnar crystals to nanocrystals. The hardness and interfacial adhesion of the gradient coatings showed a tendency of firstly increasing and then decreasing with the increase of both bias voltage and arc current. When the bias voltage and arc current are -80 V and 160 A respectively, the coating has the best mechanical properties, its surface hardness reaches 36.94 GPa, and the interfacial adhesion exceeds 120 N. In addition, with the increase of bias voltage and arc current, particles are deposited on the surface of the coating with higher energy, which leads to the preferential orientation transition from (111) to (200) plane. The high hardness of TiAlSiN coating is mainly due to the formation of high Al content of fcc-TiAlN crystals and amorphous Si3N4 in the gradient-coated surface layer. The results have important theoretical and practical significance for developing new high-performance gradient coating tools.