Previous studies are primarily based on surface air pollution for a single event, leaving research on the temporal characteristics of aerosols and wind fields in the atmospheric boundary layer (ABL) and their associations unclear due to a lack of long-term vertical profile data. This study was the first to conduct long-term Doppler wind LiDAR measurements from Sep. 2019 to Aug. 2022 in Hefei in western Yangtze River Delta (YRD) region, China. The spatiotemporal characteristics of retrieved aerosol backscatter coefficient (β) and wind profiles were analyzed from the perspective of long-term statistics and typical heavy pollution episodes (HPEs). The seasonal profile of β showed a peak in the near-surface layer meanwhile the overall β profile (<0.5 km) was the highest in winter but lowest in summer. Combined with ground-based meteorological and air quality observations, 12 HPEs were identified and classified into dust-related events and fog-haze episodes. The results showed a consistency between hourly variations in PM10 (particulate matter smaller than 10 μm) concentration and β retrieved at 300 m during a high PM10 concentration (>150 μg/m3) period. Different roles of horizontal wind at different altitudes and its associated time delay effect on surface PM10 pollution were evaluated based on correlation coefficients (Ф) and air pollution diffusion conditions. Significant positive Ф values were noticed below 0.5 km during the entire dust-related EP4 and EP6, indicating that the higher wind speeds could exacerbate PM10 pollution. In contrast, large negative Ф values meant the removal of PM10 pollutants by strong winds below 0.8 km during 24 h after peak in EP3. Combining with backward trajectory analysis and meteorological condition, notable transboundary pollution with positive contributions from upper winds (>1.5 km) was discovered in dust-related EP1, EP4, EP7, EP9, and EP10. Time delay effect (1-h/2-h lag) of upper winds (>0.8 km) on surface PM10 pollution was explored in EP5, EP6, EP7, EP8, and EP9. In spring dust-related HPEs, surface PM10 pollution was mostly contributed by long-range transport of aerosol particles at higher altitudes (>1.5 km) from the northwest direction, driven by the Mongolian cyclone and the cold front system. Transboundary aerosols originated from the northern part of Anhui province and the YRD region in the middle altitudes (∼0.5 km) was the main contributor to fog-haze HPEs. The findings demonstrated the ability of the real-time Doppler wind LiDAR system to monitor transboundary air pollution and provided a scientific reference for policy makers.