It is of great engineering significance to study methods for processing and preparing ultra-hard brittle materials with low processing cost and high processing efficiency. In this paper, the traditional Electrical Discharge Machining (EDM) ultra-hard brittle materials technology is improved, a method for processing the ultra-hard brittle materials by spray electrochemical method is proposed, and this method is applied to the processing of a typical ultra-hard brittle material monocrystalline silicon, and then the influence of processing peak voltage, pulse width/interval, electrolyte concentration and other parameters on the processing effect of the ultra-hard brittle materials is analyzed. Ultra-hard brittle materials can be etched by electrochemical etching and chemical dissolution. In this study, the conventional EDM-electrochemical technology is improved, and the liquid electrolyte is converted into a fog state by using an atomization device. The interrupted ratio of the metal wheel is set to ?=0.55; the thickness is set to 2 mm, and the rotate speed is set to 1800 r/min. The test results show that the larger the peak voltage, the larger the pulse width, the smaller the pulse interval, the larger the metal wheel rotate speed, and the larger the removal rate and surface roughness of the ultra-hard brittle material. The removal rate and surface roughness of the ultra-hard brittle material both decreased first and then increased with the increase of the electrolyte concentration. The research conclusions can provide a theoretical reference for the electrochemical processing of ultra-hard brittle materials.