Nature provides numerous examples of high-performance composites that combine organic and inorganic materials. Biological structures, such as nacre and the structural elements of glass sponges, exhibit a remarkable fracture toughness due to their layered architecture, which promotes crack de flection. This study applies a similar approach into the fiber-matrix interface in carbon fiber rein forced concrete (CFRC) by developing brick-and-mortar (BnM) or layer-by-layer (LbL) structures to mitigate brittle composite failure. Cost-effective materials, including nanoclays, sodium water glass (WG), and polymer dispersions were selected for this purpose. Montmorillonite (MMT) and polymer were used to generate self-assembled BnM structures, while LbL structures were formed through alternating layers of sodium water glass and polymer. The morphology of the developed coatings was characterized using scanning electron microscopy and energy-dispersive X-ray spectroscopy. Micro mechanical pull-out tests on individual carbon fibers embedded in concrete with BnM-and LbL-coatings demonstrated increased pull-out work. Additionally, bonding behavior was investigated using the yarn pull-out (YPO) test, revealing improved performance of the layered polymer-nanoclay dispersions compared to reference impregnations.