The presence of plant litter on the soil surface influences the flow of nutrients, carbon, water, and energy in terrestrial ecosystems. Quantifying plant litter cover is important for interpreting vegetated landscapes and for evaluating the effectiveness of conservation tillage practices. Current methods of measuring litter cover are subjective, requiring considerable visual judgment. Reliable and objective methods are needed. The spectral reflectance (0.4-2.5 μm) of wet and dry soils (six types) and plant litters (2 crops, 14 forest, and 2 grasses) of different ages were measured. Discrimination of plant litters from the soils was ambiguous in the visible and near-infrared (0.4-1.1μm) wavelength region. An absorption feature associated with cellulose and lignin was observed at 2.1 μm in the spectra of dry plant litter, which was not present in the spectra of soils. A new spectral variable, cellulose absorption index (CAI), was defined using the relative depth of the reflectance spectra at 2.1 μm. CAI of dry litter was significantly greater than CAI of soils. CAI generally decreased with age of the litter. Water absorption dominated the spectral properties of both soils and plant litter and significantly reduced the CAI of the plant litters. Nevertheless, the CAI of wet litter was significantly greater then CAI of wet soil. This study provides a new methodology to discriminate plant litter from soils by differences in spectral reflectance produced by their physical and chemical attributes. This remote sensing method should improve quantification of plant litter cover and thus improve estimates of phytomass production, surface energy balance, and the effectiveness of soil conservation practices. Plant litter reflectance is a verifiable component in vegetative landscapes and should be labeled and modeled separately from soils in landscape studies.