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Cement-based materials are widely used to build important civil infrastructures including bridges, dams, underground pipelines, skyscrapers and nuclear containments. Thus, improving the performance of cementitious materials is of great importance for constructing safe, durable, low maintenance and environment friendly infrastructure systems. Among many strategies and methods, the concept of using additives to tailor or enhance the physical, mechanical and transport properties of concrete, as well as the smartness of self-sensing and self-healing, has been widely explored. Nano-sized additives can enhance the smartness of cementitious materials. Utilizing their unique electrical properties, nano-sized additives are able to change the electrical conductivity and piezoresistive characteristics of concrete so as to enhance the sensitivity of concrete to stress and damage. Thus, smart concrete capable of self-monitoring and self-sensing can be produced when suitable nanosized additives are added into concrete; of these nanomaterials, carbon structure nanoparticles have been gaining attention as a possible material used to reinforce cementitious composites.