Vegetation indices are calculated from reflectance data of discrete spectral bands. The reflectance signal in the visible spectral range is dominated by the optical properties of photosynthetic pigments in plant leaves. Numerous spectral indices have been proposed for the estimation of leaf pigment contents, but the efficacy of different indices for prediction of pigment content and composition for species-rich communities is unknown. Assessing the ability of different vegetation indices to predict leaf pigment content we identify the most suitable spectral indices from an experimental dataset consisting of field-grown high light exposed leaves of 33 angiosperm species collected in two sites in Mallorca (Spain) with contrasting leaf anatomy and pigment composition. Leaf-level reflectance spectra were recorded over the wavelength range of 400 -900 nm and contents of chlorophyll a, chlorophyll b, total carotenoids, and anthocyanins were measured in 33 species from different plant functional types, covering a wide range of leaf structures and pigment content, fivefold to more than 10-fold for different traits. The best spectral region for estimation of leaf total chlorophyll content with least interference from carotenoids and anthocyanins was the beginning of near-infrared plateau well beyond 700 nm. Leaves of parallel-veined monocots and pinnate-veined dicots had different relationships between vegetation indices and pigments. We suggest that the nature and role of Bfar-redĉ hlorophylls which absorb light at longer wavelengths than 700 nm constitute a promising target for future remote sensing studies.