Previous studies on the calcitic seminacre of the craniid brachiopod NoVocrania have never fully resolved the crystallography of its constituent calcite crystals. With this aim, we studied the tablets forming the foliated-like and seminacre layers of this brachiopod by means of scanning electron microscopy coupled to electron backscatter diffraction. In both cases, tablets are monocrystalline and have a common crystallographic structure. Their c axes lie approximately parallel to the shell surface, and, for those tablets forming the internal shell ribs, they are also parallel to the rib elongation. There is no consistency in the orientation of the a axes in the different plates. Crystal competition processes appear to be responsible for this fiber texture. The tablets are bounded by planar rhombohedral faces. The main, innermost surface is not a crystal face but marks the boundary of the crystal with the mantle epithelium. Our data also show that, during spiral growth, the crystal axes of seminacre tablets remain stationary. Calcite twins occasionally develop in the species NoVocrania anomala. The foliated-like and seminacre microstructures are crystallographically dissimilar to the foliated layer of molluscs but similar to the foliated layer of bryozoans. The relationship of brachiopod seminacre to the molluscan nacre is also discussed.