Atmospheric acidic deposition has been a major environmental problem since the industrial revolution. However, our understanding of the effect of acidic deposition on soil pH is inconclusive. Here we examined temporal variations in topsoil pH and their relationships with atmospheric sulfur and nitrogen deposition across China’s forests from the 1980s to the 2000s. To accomplish this goal, we conducted artificial neural network simulations using historical soil inventory data from the 1980s and a data set synthesized from literature published after 2000. Our results indicated that significant decreases in soil pH occurred in broadleaved forests, while minor changes were observed in coniferous andmixed coniferous and broadleaved forests. The magnitude of soil pH change was negatively correlated with atmospheric sulfur and nitrogen deposition. This relationship highlights the need for stringent measures that reduce sulfur and nitrogen emissions so as to maintain ecosystem structure and function.