Abstract The forest floor was shown to be an effective sink of atmospherically deposited methylmercury (MeHg) but less for total mercury (Hg total ). We studied factors controlling the difference in dynamics of MeHg and Hg total in the forest floor by doubling the throughfall input and manipulating aboveground litter inputs (litter removal and doubling litter addition) in the snow‐free period in a Norway spruce forest in NE Bavaria, Germany, for 14 weeks. The MeHg concentrations in the forest‐floor percolates were not affected by any of the manipulation and ranged between 0.03 (Oa horizon) and 0.11 (Oi horizon) ng Hg L –1 . The Hg total concentrations were largest in the Oa horizon (24 ng Hg L –1 ) and increased under double litterfall (statistically significant in the Oi horizon). Similarly, concentrations of dissolved organic C (DOC) increased after doubling of litterfall. The concentrations of Hg total and DOC correlated significantly in forest‐floor percolates from all plots. However, we did not find any effect of DOC on MeHg concentrations. The difference in the coupling of Hg total and MeHg to DOC might be one reason for the differences in the mobility of Hg species in forest floors with a lower mobility of MeHg not controlled by DOC.