Dendrochronological studies and forest inventory surveys have reported increased growth and biospheric carbon (C) sequestration for European forests in the recent past. The potential of concomitant changes in forest soil C stocks are not accounted for in the IPCC guidelines for national greenhouse gas inventories. We developed a model-based approach to address this problem and assess the role of soils in forest C balance in the European Alps. The decomposition model FORCLIM-D was driven by long-term (that is, 1900–1985 AD) litter input scenarios constructed from forest inventory data, region-specific dendrochronological basal area indices, and time series of anthropogenic litter removal. The effect of spatial climate variability on organic matter decomposition across the case study region (Switzerland) was explicitly accounted for by constant long-term annual means of actual evapotranspiration and temperature. Uncertainties in forest development, litter removal, fine root litter input, and dynamics of forest soil C were studied by an explorative factorial sensitivity analysis. We found that forest soils contribute substantially to the biospheric C sequestration for Switzerland: Our ‘‘best estimate’’ yielded an increase of 0.35 Mt C/y or 0.33 t C/(ha y) in forest soils for 1985, that is, 27% of the C sequestered by forest trees (BUWAL 1994). Uncertainties regarding C accumulation in forest soils were substantial (0.11–0.58 Mt C/y) but could be reduced by estimating forest soil C stocks in the future. Whereas soils can be important for the C balance in naturally regrowing forests, their C sequestration is negligible (less than 5%) relative to anthropogenic CO2 emission in Western Europe at present.