The mineralized tissue of intertubular dentin is a collagen-mineral composi
te with considerable local variations of mechanical properties. Area scans
of human coronal dentin were made by complementary methods to investigate c
orrelations between local mechanical properties and the density, size, and
crystallinity of the mineral particles. Scanning images from the same speci
men were collected with Fourier-transform infrared microspectroscopy in ref
lectance mode (FTIR-RM), small angle X-ray scattering (SAXS), quantitative
backscattered electron imaging (qBEI), and Nanoindentation in an atomic for
ce microscope. The mineral content of dentin was found to decrease and the
thickness of mineral crystals to increase towards the dentin-enamel junctio
n (DEJ). Hardness and elastic modulus both decreased towards the DEJ. In a
correlation analysis, the mineral content and, even more, the thickness of
mineral crystals were found as the best predictors of hardness. The dentin
layer close to the DEJ corresponds to a local minimum in hardness and elast
ic modulus, a configuration known to be an effective obstacle for crack pro
pagation. Hence, the observed variations of mechanical and structural prope
rties in an area between 0 and 1.5 mm below the DEJ define crown dentin as
a gradient material optimized for its mechanical function.