The application range of potassium dihydrogen phosphate (KDP) crystals can be expanded by enhancing their surface quality properties. Therefore, a method for controlling the surface-temperature field of various materials was developed to expand the plastic zone to overcome the difficulty in processing KDP crystals. The ductile/brittle transition depth of the KDP crystals was determined using a 38 nm nanoindentation experiment. The nanoscratch experiment revealed the rules of how the transformation depth of the KDP crystals changes with temperatures, and the effect of temperature on the microstructure of the KDP crystals was studied. Finally, KDP crystal surfaces were processed using a UPDFC machine at elevated temperatures. According to our experiments, the surface roughness of the KDP crystal reached 5.275 nm as temperature increased, thus enhancing its surface quality. This method could be applied to other brittle materials.