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Urban air pollution has become a regional environmental problem. In order to explore whether island areas were affected by the urban development of surrounding areas, in this paper, we systematically study the vertical distribution characteristics of atmospheric components, meteorological drivers, potential pollution sources, and the population health risks of fine particulate matter in island cities in China. The vertical profiles of three atmospheric pollutants (aerosols, NO2, and HCHO) in the lower troposphere of Huaniao Island in the East China Sea (ECS) were obtained using ground-based multi-axial differential optical absorption spectroscopy (MAX-DOAS). The results show that the aerosol extinction coefficients, NO2, and HCHO were primarily distributed at altitudes below 1 km, and the atmospheric pollutants in Zhoushan were obviously affected by high-altitude transfer. The main meteorological driving factors of aerosols, NO2, and HCHO were different at different altitudes. The key factor contributing to the high column concentrations of NO2 and HCHO in the upper air (greater than 400 m) was the transport of pollutants brought about by changes in wind speed. By exploring the main potential sources of atmospheric pollutants, it was found that the main sources of aerosols, NO2, and HCHO are coastal cities in the Yangtze River Delta, including southeast Zhejiang Province, southeast Fujian Province, Shanghai, ECS, and the Yellow Sea. Compared with aerosols and HCHO, local primary emissions are an important source of NO2, which are mainly related to industrial activities in Zhoushan Port. In addition, using the expose-response function model, the number of attributable cases of PM2.5 air pollution in Zhoushan City in 2019 accounted for 6.58% of the total population. This study enriches our understanding of the vertical distribution characteristics of atmospheric composition and health risk assessment on Chinese islands. [ABSTRACT FROM AUTHOR]