Three-dimensional electrolysis treatment of wastewater has unique advantages in cleanliness and efficiency. This work was aimed at investigating the application of three-dimensional electrolysis in treatment of Crystal Violet (CV) wastewater. Firstly, the five single factors which consist of applied voltage, electrolysis time, electrolyte concentration, pH value in the system and the aeration rate for the impact on reduction efficiency of COD were systematically studied. The influence of these factors on COD degradation and the optimum operation conditions of electrolysis were found. The orthogonal test was carried out to determine the interaction effect of five single factors: electrolysis time > pH > external voltage > electrolyte concentration > aeration rate. The optimal experimental electrolysis conditions were determined: the pH was 5, the voltage was 14 V, aeration rate was 50 L/h, Na2SO4 electrolyte concentration was 0.15 mol/L, and the electrolysis time was 120 min. Since CV wastewater is common in printing and dyeing industry, this study highlights the potential of the three-dimensional treatment in wastewater treatment. This method has great advantages in both energy saving and high efficiency.