The effect of electrolysis operating parameters on the removal efficiency of cadmium from a simulated wastewater was studied by adopting response surface methodology combined with Box–Behnken Design. As a new electrode design, spiral-wound woven wire mesh rotating cylinder electrode was used for cadmium removal. Current (240–400 mA), rotation speed (200–1000 rpm), initial cadmium concentration (200–600ppm), and cathode mesh number (30–60) were chosen as independent variables while the removal efficiency of cadmium was considered as a response function. The results revealed that the rotation speed has the major effect on the removal efficiency of cadmium. Regression analysis showed good fit of the experimental data to the second-order polynomial model with a coefficient of determination (R2) value of 0.9931 and Fisher F-value of 89.82. The optimal conditions within the experimental ranges of the independent variables were a current of 345 mA, a rotation speed of 800 rpm, an initial cadmium concentration of 500 ppm, and a mesh number of 30, where concentration of cadmium was diminished from 500 to 8 ppm after 60 min of electrolysis with a specific energy consumption of 3.12 kWh kg−1 and a current efficiency of 41%.