Human inputs of pollutants to the atmosphere and subsequent deposition may decrease pH in the coastal waters. Significant rate of decrease in pH and increase in pCO2 by 3 to 5 times is noticed in the coastal Bay of Bengal (BoB) than the global trend in the last few decades. We provide evidence for the first time for a rapid decrease in surface water pH due to atmospheric deposition of pollutants in the coastal BoB. The decrease in pH in the coastal BoB over the last decade is associated with concomitant increase in aerosol optical depth (AOD), total suspended particles (TSP) in air, sulphate and nitrate concentrations in TSP. This study suggests that contamination of surface coastal BoB by atmospheric pollutants not only acidifies surface ocean but also potentially amplifies CO2 emission with immediate implications to regional weather and climate.