Atmospheric aerosol is one of the major factors that cause environmental pollution. Light detection and ranging (LiDAR) is an effective remote sensing tool for aerosol observation. In order to provide a comprehensive understanding of the aerosol pollution from the physical perspective, this study investigated regional atmospheric aerosol pollution through the integration of measurements, including LiDAR, satellite, and ground station observations and combined the backward trajectory tracking model. First, the horizontal distribution of atmospheric aerosol wa obtained by a whole-day working scanning micro-pulse LiDAR placed on a residential building roof. Another micro-pulse LiDAR was arranged at a distance from the scanning LiDAR to provide the vertical distribution information of aerosol. A new method combining the slope and Fernald methods was then proposed for the retrieval of the horizontal aerosol extinction coefficient. Finally, whole-day data, including the LiDAR data, the satellite remote sensing data, meteorological data, and backward trajectory tracking model, were selected to reveal the vertical and horizontal distribution characteristics of aerosol pollution and to provide some evidence of the potential pollution sources in the regional area. Results showed that the aerosol pollutants in the district on this specific day were mainly produced locally and distributed below 2.0 km. Six areas with high aerosol concentration were detected in the scanning area, showing that the aerosol pollution was mainly obtained from local life, transportation, and industrial activities. Correlation analysis with the particulate matter data of the ground air quality national control station verified the accuracy of the LiDAR detection results and revealed the effectiveness of LiDAR detection of atmospheric aerosol pollution.