Urban Heat Island (UHI) and Urban Pollution Island (UPI) are two major problems of the urban environment and have become more serious with rapid urbanization. Since UHI and UPI can interact with each other, these two issues should be studied concurrently for a better urban environment. This study investigated the interaction between the UHI and UPI in Berlin, through a combined analysis of in-situ and remote sensing observations of aerosols and meteorological variables in June, July, and August from 2010 to 2017. The atmospheric UHI (AUHI), surface UHI (SUHI), atmospheric UPI (AUPI), and near-surface UPI (NSUPI) were analyzed. The SUHI and AUPI are represented by the remote sensing land surface temperature (LST) and aerosol optical depth (AOD), and the AUHI and NSUPI are represented by the in-situ air temperature and Particulate Matter (PM10) concentrations. The study area shows spatial consistency between SUHI and AUPI, with higher LST and AOD in the urban areas. UHI strengthens the turbulent dispersion of particles in the urban areas, decreasing the NSUPI. The NSUPI intensity shows a negative relationship with the AUHI intensity, especially at night with a correlation coefficient of −0.31. The increased aerosols in urban atmosphere reduce the incoming solar radiation and increase the atmospheric longwave radiation in the urban areas. The response of the surface to the change of absorbed radiation is strong at night and weak during the day. This study estimates that the SUHI intensity is enhanced by around 12% at clear night by the increased absorbed radiation in the urban areas using an attribution method. The goal of this paper is to strengthen the understanding of the interactive influence between UHI and UPI and provide a basis for designing mitigation strategies of UHI and UPI. © 2018 Elsevier B.V.