During the last decades, forest soils in Central Europe recovered from former sulfur and acid deposition. As external S input into forests has strongly decreased and legacy S pools in the soils are diminishing, internal S cycling through mineralization will increasingly become important for ecosystem nutrition. However, it is not known how microbial biomass is affected by the S pool change in the formerly S surplus soils. Here, we present data on the status quo of C, N, and S in microbial biomass in relation to contents in mineral soil and organic layer. The results of forest soil in Eastern Germany (low and high liming), which is slowly recovering from former pollution, are compared to those of a site remote from air pollution in the Swiss Alps. The contents of C, N, and S in soil as well as in microbial biomass were clearly higher in the organic layer than in mineral topsoil at all sites. Despite the generally low content in the mineral A-horizon, the clean-air site showed indications of a more active S-turnover as compared to the high-pollution site. Liming at the high-pollution site improved the conditions for microbial growth (pH increase) in the organic layer resulting in more mobile S.