Brachiopod shells consist of low-magnesium calcite and belong to one of the most intriguing species for studies of marine paleoenvironments, variations in oceanographic conditions and ocean chemistry [6, 7, 11 – 13]. We have investigated the ultrastructure together with nano- and microhardness properties of modern brachiopod shells with transmission electron microscopy (TEM), scanning electron microscopy (SEM), nanoindentation and Vickers microhardness analyses. Brachiopod shells are structured into several layers, a thin, outer, hard, protective primary layer composed of randomly oriented nanocrystalline calcite, which is followed inward towards the soft tissue of the animal by a much softer shell segment (secondary layer) built of long calcite fibres, stacked parallely into blocks. The hardness distribution pattern within the shells is non-uniform and varies on scales as small as a few tens of microns. Our results show that the hardness of this biomaterial is controlled by two predominant features: (1.) The morphological orientation of the calcite fibres (not by the crystallographic orientation of the fibres), and (2.) the amount and distribution pattern of organic material between and within the calcite crystals.