Air pollution has emerged as a significant health, environmental, economic, and social problem all over the world. In this study, geospatial technologies coupled with a LUR (Land Use Regression) approach were applied to assess the spatial-temporal distribution of fine particulate (PM2.5). In-situ observations of air pollutants from ground monitoring stations from 2016–2018 were used as dependent variables, while the land-use/land cover, a NDVI (Normalized Difference Vegetation Index) from a MODIS sensors, and meteorology data allocations surrounding the monitoring stations from 0.25–5 km buffer ranges were collected as spatial predictors from GIS and remote sensing databases. A linear regression method was developed for the LUR model and 10-fold cross-validation was used to assess the model robustness. The R2 model obtained was 56% for DKI Jakarta, Indonesia, and 83% for Taipei Metropolis, Taiwan. According to the results of the PM2.5 model, the essential predictors for DKI Jakarta were influenced by temperature, NDVI, humidity, and residential area, while those for the Taipei Metropolis region were influenced by PM10, NO2, SO2, UV, rainfall, spring, main road, railroad, airport, proximity to airports, mining areas, and NDVI. The validation of the results of the estimated PM2.5 distribution use 10-cross validation with indicated R2 values of 0.62 for DKI Jakarta and 0.84 for Taipei Metropolis. The results of cross-validation show the strength of the model.