Since the middle of the last century, global surface air temperature exhibits an increasing trend, with nocturnal temperatures increasing at a much higher rate. Proposed causative mechanisms include the radiative impact of atmospheric aerosols on the nocturnal boundary layer (NBL) where the temperature response is amplified due to shallow depth and its sensitivity to potential destabilization. A 1-D version of the Regional Atmospheric Modeling System is used to examine the sensitivity of the nocturnal boundary layer temperature to the surface longwave radiative forcing (SLWRF) from urban aerosol loading and doubled atmospheric carbon dioxide concentrations. The analysis is conducted for typical midlatitude nocturnal boundary layer case days from the CASES-99 field experiment and is further extended to urban sites in Pune and New Delhi, India. For the cases studied, locally, the nocturnal SLWRF from urban atmospheric aerosols (2.7–47 W m−2) is comparable or exceeds that caused by doubled atmospheric carbon dioxide (3 W m−2), with the surface temperature response ranging from a compensation for daytime cooling to an increase in the nocturnal minimum temperature. The sensitivity of the NBL to radiative forcing is approximately 4 times higher compared to the daytime boundary layer. Nighttime warming or cooling may occur depending on the nature of diurnal variations in aerosol optical depth. Soil moisture also modulates the magnitude of SLWRF, decreasing from 3 to 1 W m−2 when soil saturation increases from 37% to 70%. These results show the importance of aerosols on the radiative balance of the climate system.