Liming has been used to mitigate effects of acidic deposition in forest ecosystems. This study was designed to examine the effects of calcium (Ca) supply on the spatial patterns and the relations between soil and soil solution chemistry in a base-poor forest watershed. Watershed 1 at the Hubbard Brook Experimental Forest in New Hampshire, USA was experimentally treated with wollastonite (CaSiO3) in October, 1999. Exchangeable Ca (Ex-Ca), soil pHs (in 0.01 M CaCl2), effective cation exchange capacity (CECe), and effective base saturation (BSe) increased, while exchangeable acidity (Ex-Acid) decreased in organic soil horizons in 2000 and 2002. Mineral soils experienced either small increases in Ex-Ca, pHs, CECe, BSe, small decreases in Ex-Acid or no changes. Thus, most of the added Ca remained in the forest floor during the study period. Prior to the treatment the BSe decreased with increasing elevation in organic and mineral soil horizons. This spatial pattern changed significantly in the forest floor after the treatment, suggesting that soils at higher elevations were more responsive to the chemical addition than at lower elevations. Soil solutions draining the forest floor responded to the treatment by increases in concentrations of Ca, dissolved silica, pH, and acid neutralizing capacity (ANC), and a decrease in inorganic monomeric Al (Ali). Treatment effects diminished with increasing soil depth and decreasing elevation. Positive correlations between Ca/total monomeric Al (Alm) in soil solution and Ex-Ca/Ex-Al ratios in soil indicated that changes in the chemistry of soils significantly influenced the chemistry of soil water, and that Ca derived from the dissolution of wollastonite mitigated the mobilization of Al within the experimental watershed.