The nano-engineered cementitious composites (NCC) were prepared using g-C3N4/CoAl-LDH nanoflower (nano-CN/L), in combination with mineral admixtures including fly ash (FA), metakaolin (MK), and ground granulated blast furnace slag (GGBFS). The synergistic effects and mechanisms of nano-CN/L and mineral admixtures on the mechanical, chloride penetration resistance and air purification properties of NCC were investigated. The results show that nano-CN/L promotes the early hydration of cementitious materials and improves the composition and morphology of C-S-H gel. Furthermore, the filling effect of nano-CN/L significantly optimizes the pore structure and interfacial crack width of NCC, thereby eliminating the adverse impact of FA, MK, and GGBFS on its early mechanical strengths. Additionally, nano-CN/L enhances the chloride penetration resistance and NOx removal properties of NCC through its strong ion adsorption and photocatalytic activity, respectively. Incorporating 0.9 % nano-CN/L by mass of cementitious materials reduces the chloride diffusion coefficient of NCC at curing age of 56d by 26.9 % and increases the NOx removal ratio by 11 times. The 7d’s compressive and flexural strengths of NCC increase by 13.6 % and 4.6 %, respectively, compared to the one without nano-CN/L. As a novel multifunctional nanomaterial, nano-CN/L not only provides a new pathway for extending the service life of cementitious composites, but also injects new momentum into their environmental-friendly development.
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