Anisotropy in shales is becoming an important issue in exploration and reservoir geophysics. In this study, the crystallographic preferred orientation of clay platelets that contributes to elastic anisotropy was determined quantitatively by hard monochromatic X-ray synchrotron diffraction in two different shales from drillholes off the coast of Nigeria. To analyze complicated diffraction images with five different phases (illite/smectite, kaolinite, quartz, siderite, feldspar) and many overlapping peaks, we applied a methodology based on the crystallographic Rietveld method. The goal was to describe the intrinsic physical properties of the sample (phase composition, crystallographic preferred orientation, crystal structure, and microstructure) and compute macroscopic elastic properties by averaging single crystal properties over the orientation distribution for each phase. Our results show that elastic anisotropy resulting from crystallographic preferred orientation of the clay particles can be determined quantitatively. This provides a possible way to compare measured seismic anisotropy and texture-derived anisotropy and to estimate the contribution of the low-aspect ratio pores aligned with bedding.