Degraded air quality by PM 2.5 can cause various health problems. Satellite observations provide abundant data for monitoring PM 2.5 pollution. While satellite-derived products, such as aerosol optical depth (AOD) and normalized difference vegetation index (NDVI), have been widely used in estimating PM 2.5 concentration, little research was focused on the use of remotely sensed nighttime light (NTL) imagery. This study evaluated the merits of using NTL satellite images in predicting ground-level PM 2.5 at a regional scale. Geographically weighted regression (GWR) was employed to estimate the PM 2.5 concentration and analyze its relationships with AOD, meteorological variables, and NTL data across the New England region. Observed data in 2013 were used to test the constructed GWR models for PM 2.5 prediction. The Vegetation Adjusted NTL Urban Index (VANUI), which incorporates Moderate Resolution Imaging Spectroradiometer (MODIS) NDVI into NTL to overcome the defects of NTL data, was used as a predictor variable for final PM 2.5 prediction. Results showed that Defense Meteorological Satellite Program/Operational Linescan System (DMSP/OLS) NTL imagery could be an important dataset for more accurately estimating PM 2.5 exposure, especially in urbanized and densely populated areas. VANUI data could obviously improve the performance of GWR for the warm season (GWR model with VANUI performed 17% better than GWR model without NDVI and NTL data and 7.26% better than GWR model without NTL data in terms of RMSE), while its improvements were less obvious for the cold season (GWR model with VANUI performed 3.6% better than the GWR model without NDVI and NTL data and 1.83% better than the GWR model without NTL data in terms of RMSE). Moreover, the spatial distribution of the estimated PM 2.5 levels clearly revealed patterns consistent with those densely populated areas and high traffic areas, implying a close and positive correlation between VANUI and PM 2.5 concentration. In general, the DMSP/OLS NTL satellite imagery is promising for providing additional information for PM 2.5 monitoring and prediction.