Understanding the sources of chemical components in roof runoff can help to prevent water quality problems in rooftop rainwater harvesting. To identify the contribution of wet deposition to the mass of components in roof runoff, the samples from air, rainwater, dust buildup and roof runoff were collected from an urban site in Shenzhen of China in 2011–2012. The results indicate that: (1) wet deposition has a dominant contribution to the mass of total organic carbon (TOC), NH4+, NO3–, Cl– and organic acids in the roof runoff, while the mass of NH4+, acetic acid and formic acid in the roof runoff may be greatly reduced by the neutralization between the components with alkaline dust buildup on the rooftop; and (2) wet deposition partially contributes to the mass of Na+, K+, Mg2+, Ca2+, F– and SO42– in the roof runoff, while other factors like dust buildup on the rooftop and chemical reactions also have a non-negligible impact. Furthermore, TOC, NH4+, NO3– and organic acids in the wet deposition are mainly influenced by the atmospheric pollution due to fast increase in fossil fuel consumption (e.g. vehicle emissions). Therefore, the effects of wet deposition should be carefully considered for rooftop rainwater harvesting in urbanized areas.