A series of problems that are related to population, resources, environment, and ecology have emerged in recent years with the advancement of industrialization and urbanization in China. Especially, air pollution has become a severe trouble that directly endangers the health of residents. Accordingly, it is a need to make the assessment of air quality among cities, so that corresponding measures can be taken. For this purpose, ten major cities are selected as the research objects in Yangtze River Delta. Additionally, this study gathers and processes the data of five main air pollutants PM2.5, PM10, SO2, O3, and NO2, respectively. Furthermore, the maximizing deviation method is used to obtain the respective weight of these pollutants and the preference ranking organization method for enrichment evaluations (PROMETHEE) is introduced into the assessment of air quality among ten cities. As a result, the ranking of air quality in Ningbo, Wenzhou, Shanghai, and Shaoxing was at the fore from 2014 to 2017. Meanwhile, the performance of Ningbo has always kept the top two and Shaoxing’s ranking has risen since 2015. In addition, the air quality of Changzhou, Suzhou and Hangzhou was at an average level in the past four years. Moreover, the performance of Nanjing, Wuxi, and Zhenjiang was terrible when compared to other cities. Some useful suggestions have been proposed to control air quality based on the ranking results.