Segment-structured diamond-like carbon (S-DLC) film, which is separated DLC films into small segments using metal mask, has been developed in order to improve its tribological property or accomplish multi-functionalized surface. Meanwhile, the S-DLC deposition by conventional methods using metal mesh as masks is difficult to apply to the three-dimensional substrates which have complicate curves. The purpose of this study is to develop coating methods for S-DLC deposition on the three-dimensional substrates like an aspect of the cylinder and a ball surface. In this study, we report the coating method using a robot employing six degrees of freedom (MOTOMAN-MH6: Yaskawa electric corporation) and a micro ink jet system (IJHB-1000 and IJHB-30: Microjet corporation). By adjusting the parameters applied to the piezoelectric element, the ink droplet was stable discharged. Then, small grid patterns were drawn on the plate. The substrate temperature is also controlled in order to make the drawn line thinner, because the resin ink is thermosetting material. Then, the DLC film was deposited onto the ink drawn substrate by a micro-pulse plasma CVD method using acetylene gas for 40 minutes. After the liftoff and the Raman spectroscopy measurement, we found that the resin ink could play a role as a mask material. Finally, grid patterns were successfully drawn on the aspect of the cylinder and a ball surface. In conclusion, it could be thought that this masking method could be used to various shape by complicating the robot programming in the future.