Dissolved organic matter in soils can be predicted from forest floor C:N ratio, which in turn is related to foliar chemistry. Little is known about the linkages between foliar constituents such as chlorophylls, lignin, and cellulose and the concentrations of water-extractable forest floor dissolved organic carbon and dissolved organic nitrogen. Lignin and cellulose are not mobile in foliage and thus may be indicative of growing conditions during prior years, while chlorophylls respond more rapidly to the current physiological status of a tree and reflect nutrient availability. The aim of this study was to examine potential links among spectral foliar data, and the organic C and N of forest soils. Two coniferous species (red spruce and balsam fir) were studied in the White Mountains of New Hampshire, USA. Six trees of each species were sampled at 5 watersheds (2 in the Hubbard Brook Experimental Forest, 3 in the Bartlett Experimental Forest). We hypothesized that in a coniferous forest, chemistry of old foliage would better predict the chemical composition of the forest floor litter layer than younger foliage, which is the more physiologically active and the most likely to be captured by remote sensing of the canopy. Contrary to our expectations, chlorophyll concentration of young needles proved to be most tightly linked to soil properties, in particular water-extractable dissolved organic carbon. Spectral indices related to the chlorophyll content of needles could be used to predict variation in forest floor dissolved organic carbon and dissolved organic nitrogen. Strong correlations were found between optical spectral indices based on chlorophyll absorption and forest floor dissolved organic carbon, with higher foliage chlorophyll content corresponding to lower forest floor dissolved organic carbon. The mechanisms behind these correlations are uncertain and need further investigation. However, the direction of the linkage from soil to tree via nutrient availability is hypothetized based on negative correlations found between foliar N and forest floor dissolved organic carbon.