Fluid jet polishing is an emerging process which possesses the advantages of localized force and less heat generation, as well as the stable and controllable material removal function without tool wear. Due to the complex machining mechanism, it is still difficult to model the material removal rate and predict the surface generation for fluid jet polishing. In this article, theoretical and experimental investigation of three-dimensional-structured surface generation by fluid jet polishing has been carried out. A surface topography simulation model is established for predicting the three-dimensional-structured surface generation by fluid jet polishing. A series of polishing experiments have been conducted to optimize the process parameters of fluid jet polishing and the fabrication of three-dimensional-structured surfaces. In terms of the pattern of three-dimensional-structured surfaces generated, the simulation results are found to agree with the experimental results.