The rapid development of image technology and optical network technology requires novel electronic and optical devices of small size and complex surfaces but well-controlled surface morphology and quality. [1] One representative example is the aspheric lens that has been widely used in digital image products due to its superior performance. [2] Currently, most aspheric lenses are manufactured by cemented carbide molds following a traditional process. [3] The molds should have accurate geometric dimensions and excellent surface smoothness. Therefore, a precision polishing process is essential to improve the surface quality of the mold. Traditionally, polishing pad and grinding head are used for the polishing work, with abrasive particles added between the workpiece and the polishing pad. [4] This approach will generate nonuniform contact forces on the workpiece surface due to the accumulation of abrasive particles, thereby affecting the efficiency and uniformity in the polishing process. In addition, the polishing wheel is not small enough for polishing mold of microscale sizes due to the limitation of machine tool and tool size. To overcome the drawbacks of the traditional contact polishing method with fixed abrasive particles, it is highly demand to explore new advanced polishing approaches that can continuously gather abrasive particles into the polishing area for a long time to achieve constant material removal rate. Electrorheological (ER) fluid is a smart material that can be controlled to change the rheological property and viscosity reversibly under an external electric field. [5-9] The rheological behaviors can be easily altered with the application of an electric field and return to its original viscosity when the electric field is removed. [10] The ER fluid generally consists of two phases: solid particles with good dielectric properties as the dispersed phase and non-conducting liquids as the continuous phase. [11] The dispersed particles are usually inorganic materials that have high dielectric constants and strong polarization properties. However, the liquid continuous phase has a relatively lower permittivity and insulation properties. Without electric field, the dispersed particles are freely suspended in the continuous fluid phase, exhibiting properties similar with Newtonian fluids. After an electric field is applied, the dispersed solid particles will be polarized, thereby forming particle chains along the direction of the applied electric field and transforming into a Bingham fluid state. [12-14] ER fluid has been explored for polishing processing of precision products. For example, Kaku et al. and Kuriyagawa et al. first mixed ultra-fine abrasives particles into the ER fluid to show almost the same rheological property as ER particles and applied the ER fluid with diamond, Al 2 O 3 , or SiC particles for optical microlenses. [2,15] Following that, extensive studies investigated the performance of electrorheological fluid-assisted polishing (ERFP), including the behavior of dispersed particles,...