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In order to solve the problem of precise control of droplet diameter variables during aviation spray, the quadratic regression orthogonal experiment and machine learning was used to establish the quadratic residual compensation droplet diameter model. With Aerial-E electricity atomizer as the control object, the quadratic regression orthogonal experiment was carried out on the atomization experiment platform to analyze the correlation between the droplet diameter and the wind speed, flow rate, atomizer speed, and droplet diameter model was established. In order to improve the prediction accuracy, a compensation factor was added to establish the first optimized droplet diameter compensation model. To further improve the prediction accuracy, the second residual prediction model was established by machine learning, the second residual prediction model and the first optimized droplet diameter compensation model were superimposed linearly to obtain the quadratic residual compensation droplet diameter model. In order to verify the validity of the quadratic residual compensation droplet diameter model, the model validation experiment and the comparative experiment were carried out, the results showed that the maximum deviation predicted by the quadratic residual compensation droplet diameter model was 10.78%, the R2 between the predicted and measured values of the quadratic residual compensation droplet diameter model was 0.95, which was 0.06 higher than that of the droplet diameter model and 0.05 higher than that of the first optimized droplet diameter compensation model. The quadratic residual compensation atomization model of electricity atomizer was obtained by equivalent deformation of the quadratic residual compensation droplet diameter model, and an electricity atomization system was designed based on the model. A system application experiment was carried out to verify the practicality of the system, the results showed that the R2 between the expected and the measured value of the droplet diameter was 0.94, and the relative span of droplet was less than 1.6, which could realize the control of the droplet diameter under the condition of stable wind speed and flow rate. The results can realize precise control of droplet diameter variables during aviation spray. 