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The comprehensive effects of anthropogenic aerosols (sulfate, black carbon, and organic carbon) on terrestrial aridity were simulated using an aerosol-climate coupled model system. The results showed that the increase in total anthropogenic aerosols in the atmosphere from 1850 to 2010 had caused global land annual mean precipitation to decrease by about 0.19 (0.18, 0.21) mm day(-1), where the uncertainty range of the change (minimum, maximum) is given in parentheses following the mean change, and reference evapotranspiration ET0 (representing evapotranspiration ability) to decrease by about 0.33 (0.31, 0.35) mm day(-1). The increase in anthropogenic aerosols in the atmosphere from 1850 to 2010 had caused land annualmean terrestrial aridity to decrease by about 3.0% (2.7%, 3.6%). The areal extent of global total arid and semiarid areas had reduced due to the increase in total anthropogenic aerosols in the atmosphere from preindustrial times. However, it was found that the increase in anthropogenic aerosols in the atmosphere had enhanced the terrestrial aridity and thus resulted in an expansion of arid and semiarid areas over East and South Asia. The projected decrease in anthropogenic aerosols in the atmosphere from 2010 to 2100 will increase global land annual mean precipitation by about 0.15 (0.13, 0.16) mm day(-1) and ET0 by about 0.26 (0.25, 0.28) mm day(-1), thereby producing a net increase in terrestrial aridity of about 2.8% (2.1%, 3.6%) and an expansion of global total arid and semiarid areas.