The present study aims to investigate the relationship between reduced air pollution and ecosystem services in Karaj metropolis, Iran. To the end, the trends in the concentrations of O3, NO2, CO, SO2, PM10, and PM2.5 as the main atmospheric pollutants of Karaj were studied. Five time series models of autoregressive (AR), moving average (MA), autoregressive moving average (ARMA), autoregressive integrated moving average (ARIMA), and seasonal autoregressive integrated moving average (SARIMA) were used to predict changes in air pollutant concentrations. Air pollution zoning is conducted via ArcGIS10.3 by using spline tension interpolation method. Then, normalized difference vegetation index (NDVI) was obtained from Landsat Thematic Mapper (TM) and Operational Land Imager (OLI) images to analyze vegetation dynamics as an index of ecosystem functioning. NDVI thresholds were selected to present guidelines for qualitative and quantitative changes in green cover and were divided into five different categories. Based on the results, AR (1) and ARIMA (1,2,1) were recognized as appropriate models for predicting the concentration of air pollutants in the study area. A decrease in very dense vegetation coverage and increase in poor vegetation areas, followed by an increase in air pollution, revealed that the loss of urban green coverage and decreased ecosystem services were positively related. Furthermore, the expansion of urban lands toward the north and the west from the baseline to future condition led to great changes in the land cover and losses in vegetation along these axes, which finally resulted in increased air pollution in these areas. Thus, the results of this study can be directly used in decision-making in the area of air pollution.