Microstructured surfaces on hard and brittle materials are widely used in a series of scientific and industrial applications, such as micro-electro-mechanical systems, nano-electro-mechanical systems, electronic devices, and medical products. However, the efficient precision machining of microstructured surfaces on hard and brittle materials faces great challenges. In this study, a new machining technology for high-efficiency precision fabrication of microstructured surface on hard and brittle materials was developed by a microstructured coarse-grained diamond grinding wheel. Initially, the laser microstructuring of the conditioned coarse-grained diamond grinding wheel was introduced. The influence of the laser-machined microstructure geometry on the form accuracy of the final, ground microstructured surface was theoretically analysed. Subsequently, the ductile regime grinding of the microstructured surface was examined for WC cermet and BK7 optical glass. The ground surfaces mainly under the ductile regime material removal were successfully achieved, especially in the case of WC ceramic. Finally, different linear and square microstructured surfaces with high form accuracy, sharp microstructure edge, and nanoscale surface roughness were efficiently fabricated on WC and BK7 optical glass by the method developed in the study.