Nature provides various templates for integrating organic and inorganic materials to create high-performance composites. Biological structures such as nacre and the structural elements of the glass sponge are built up in layers, leading to remarkable fracture toughness. In this work, the brick-and-mortar and layer-by-layer structures found in these biological examples have been abstracted and implemented by using an aqueous polymer dispersion in combination with nanoclay particles and sodium water glass. These dispersions were used as impregnation of carbon rovings in order to form bio-inspired contact zones towards the concrete matrix. The bonding behavior was investigated using the Yarn Pull-Out (YPO) test, and a beneficial behavior of the layered polymer–nanoclay dispersions was observed. Thermogravimetric analysis (TGA) was used to determine the organic impregnation content of the roving. Further, light microscopy of the roving cross-sections prior to YPO and visual analyses of the fractured contact zone of split concrete specimens provided information on the quality of the impregnation and the interaction with the concrete matrix.