Cross-site syntheses of litter decomposition studies have shown that litter calcium (Ca) concentration may have a role in controlling the extent of decomposition of tree foliage. We used an ongoing watershed CaSiO4 addition experiment at the Hubbard Brook Experimental Forest in New Hampshire, USA, to test the hypotheses that increased Ca in litter would have no effect on the initial rates of litter decay but would increase the extent or completeness (limit value) of foliar litter decomposition. We tested these hypotheses with a 6-year litter decomposition experiment using foliar litter of four tree species that are prominent at this site and in the Northern Hardwood forest type of North America: sugar maple (Acer saccharum Marsh), American beech (Fagus grandifolia Ehrh.) yellow birch (Betula alleghaniensis Britt.) and white ash (Fraxinus americana L.). The experiment used a reciprocal transplant design with the Ca-treated watershed and a control site providing two sources of litter and two placement sites. This dataset includes mass loss and changes in nutrient content of litter over the six year period.