Summer soil moisture increased significantly from 1958 to the mid 1990s in Ukraine and Russia. This trend cannot be explained by changes in precipitation and temperature alone. To investigate the possible contribution from solar dimming and upward CO2 trends, we conducted experiments with a sophisticated land surface model. We demonstrate, by imposing a downward trend in incoming shortwave radiation forcing to mimic the observed dimming, that the observed soil moisture pattern can be well reproduced. On the other hand, the effects of upward CO2 trends were relatively small for the study period. Our results suggest tropospheric air pollution plays an important role in land water storage at the regional scale, and needs to be addressed accurately to study the effects of global warming on water resources.