Air pollution is a major environmental health problem. The study of interaction between air pollution and human will benefit to the human health and well-being of community. Both a model for assessing population relative risk of air pollution exposure (MAPRRAPE) and air pollution concentration methods were applied in a case study to determine the optimal method in evaluating risk of population exposure to Sulfur Dioxide (SO2). The framework for building the MAPRRAPE was described in detail. Then, the spatial patterns of population by demographic characteristics exposed to SO2 from industrial, vehicle, and the mixture of industrial and vehicle pollution sources, as well as an in-depth quantitative investigation using correlation analysis were studied for further source appointment. The results showed that the MAPRRAPE was more reliable than air pollution concentration model in determining population exposure risks by demographic characteristics. The high risk areas of whites exposed to SO2 were larger than blacks and the other races due to a large number of whites, and other age groups exposed to SO2 were larger than children and the old people. In addition, the correlation analyses showed that the relative risks of population by demographic characteristics exposed to SO2 had a more significant correlation with vehicle pollution source than industrial pollution source. The results of source appointment thus demonstrated that vehicle pollution source was the main pollution source. This study suggests that there is a clear need for the implementation of programs and services that will reduce population exposed to air pollution with focusing on densely populated areas for an ultimate improvement of community health status and the environmental conditions.