Coal dust is hazardous to underground coal workers and water spray is the most common and economic method for controlling coal dust. Previous studies proved that the addition of surfactants can improve the performance of water spray on coal dust suppression. The evaluation methods for surfactants vary from different studies. The zeta potential test is a common method for evaluating surfactants with ionicity. Generally, the suspension of coal dust with pure water usually showed a negative value of zeta potential. The addition of cationic surfactants can increase the zeta potential to a positive value with a small dosage, while the addition of anionic surfactants can only lower the zeta potential. However, there is a lack of comprehensive study to investigate the relationship between the zeta potential and the suppression performance for coal dust. The aim of this study is to reveal the consistency and discrepancy between the zeta potential and the suppression efficiency of a surfactant. Firstly, the mixture of cationic surfactant solutions and coal dust would be evaluated by the zeta potential test. The wind tunnel tests would then be conducted for the same surfactant solutions to measure and calculate the suppression efficiency. It was found that the addition of surfactant can increase the zeta potential and the suppression efficiency and it reached the greatest efficiency when the zeta potential approached to zero. The equilibrium of zeta potential can benefit the suppression performance of surfactants in the wind tunnel test. The result of this study can achieve a better understanding of the mechanism for coal dust suppression. The selection of surfactants will also be suggested for researchers or industries in terms of coal dust control. It would be more economic if a similar performance could be achieved by less consumption of surfactants.