To investigate the evolution of the nocturnal boundary layer (NBL) and its impacts on the vertical distributions of pollutant particulates, a combination of in situ observations from a large tethered balloon, remote sensing instruments (aerosol lidar and Doppler wind lidar) and an atmospheric environment-monitoring vehicle were utilized. The observation site was approximately 100 km southwest of Beijing, the capital of China. Results show that a considerable proportion of pollutant particulates were still suspended in the residual layer (RL) (e.g., the nitrate concentration reached 30 μg m−3) after sunset. The NBL height calculated by the aerosol lidar was closer to the top of the RL before midnight because of the pollutants stored aloft in the RL and the shallow surface inversion layer; after midnight, the NBL height was more consistent with the top of the surface inversion layer. As the convective mixing layer gradually became established after sunrise the following day, the pollutants stored in the nocturnal RL of the preceding night were entrained downward into the mixing layer. The early morning PM2.5 concentration near 700 m in the RL on 20 December decreased by 83% compared with the concentration at 13:34 on 20 December at the same height. The nitrate concentration also decreased significantly in the RL, and the mixing down of nitrate from the RL could contribute about 37% to the nitrate in the mixing layer. Turbulence activities still existed in the RL with the bulk Richardson number (Rb) below the threshold value. The corresponding increase in PM2.5 was likely to be correlated with the weak turbulence in the RL in the early morning.