Cement-based materials are strong yet brittle, organic modifications enhance their flexibility and durability, reducing cracks. The study investigates cementitious composites inspired by the “inorganic brick-and-organic mud” structure of nacre, focusing on organic modifications with Polyvinyl Alcohol (PVA) to enhance binding capacity and mechanical properties. Calculated Free energy and separation force indicate that lower organic concentrations effectively envelop inorganic surfaces, preventing organic aggregation. These organic-inorganic interactions vary with organic concentration and aqueous conditions, demonstrating notable kinetic peaks. Particularly in aqueous settings, PVA efficiently binds two otherwise separate calcium silicate hydrate (CSH) sheets, showcasing its effectiveness as a binder. The study identified a 5 % concentration of organics as optimal for effectively binding CSH sheets. The level not only enhances the mechanical properties of the composites but also significantly improves the CSH binding capacity. The free energy, separation force and mechanical properties provide vital insights into the development of advanced bio-inspired cementitious composites.