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Wastewater treatment by ozonation has the advantage of strong oxidizing ability and no secondary pollution. However, the mass-transfer resistance of the gas–liquid interface makes this process less efficient. In this work, a superaerophilic surface was introduced to solve this problem. It was confirmed that the superaerophilic surface could improve the liquid phase mass-transfer coefficient (K L) based on its super affinity to gas through the single board experiment. Moreover, aeration experiment showed that the result KL of superaerophilic packing resulted in 5.6 and 1.6 times greater values as compared to the bubbling device and the commercial aeration device. It was found that superaerophilic packing showed good performance in both simulated wastewater and actual wastewater. The decolorization time of simulated dye wastewater was shortened by 20 and 50% compared with the commercial aeration device and the bubbling device, respectively. The degradation rate of chemical oxygen demand was increased by 14% in this system. It was found that the enhancement was more obvious at a low gas flow rate and a high initial concentration of the pollutants. The stability test result showed that the prepared packing had good ozone resistance and solvent stability and can stand high temperature and hydraulic impact. This work provides a new strategy for improving gas–liquid mass-transfer efficiency and has a potential practical prospect.