Exposure to fine particulate matter (PM 2.5 ) is associated with adverse health impacts on the population. Satellite observations and machine learning algorithms have been applied to improve the accuracy of the prediction of PM 2.5 concentrations. In this study, we developed a PM 2.5 retrieval approach using machine-learning methods, based on aerosol products from the Moderate Resolution Imaging Spectroradiometer (MODIS) aboard the NASA Earth Observation System (EOS) Terra and Aqua polar-orbiting satellites, near-ground meteorological variables from the NASA Goddard Earth Observing System (GEOS), and ground-based PM 2.5 observation data. Four models, which are orthogonal regression (OR), regression tree (Rpart), random forests (RF), and support vector machine (SVM), were tested and compared in the Beijing-Tianjin-Hebei (BTH) region of China in 2015. Aerosol products derived from the Terra and Aqua satellite sensors were also compared. The 10-repeat 5-fold cross-validation (10 × 5 CV) method was subsequently used to evaluate the performance of the different aerosol products and the four models. The results show that the performance of the Aqua dataset was better than that of the Terra dataset, and that the RF algorithm has the best predictive performance (Terra: R = 0.77, RMSE = 43.51 µg/m 3 ; Aqua: R = 0.85, RMSE = 33.90 µg/m 3 ). This study shows promise for predicting the spatiotemporal distribution of PM 2.5 using the RF model and Aqua aerosol product with the assistance of PM 2.5 site data.