Nano-silica (NS) is one of the most important nanomaterials in recent years. It is used as a new cement-based composite reinforcement in building materials because of its high volcanic ash activity. In order to achieve the goal of carbon peaking and carbon neutralization, combined with the research idea of cementitious materials-reducing admixture for concrete, under the condition of reducing the amount of cement in concrete by 20%, the influence of different dosages of NS on the setting time and mechanical properties of concrete was analyzed. In addition, the shrinkage performance, impermeability, and resistance to chloride-ion permeability of concrete were also studied. The results show that under the same curing conditions and ages, when the NS dosage is 2.5%, the compressive strength and splitting tensile strength of the specimen after 28 days of curing are the highest, reaching 40.87 and 3.8 MPa, which show an increase by 6.6 and 15.15%. The shrinkage performance of concrete increases with the increase in NS dosage. In addition, when the NS dosage is 2.0%, the durability of concrete has also been greatly improved. The impermeability of concrete increased by 18.7% and the resistance to chloride-ion permeability increased by 14.7%. Through microscopic analysis it was found that NS can promote the hydration reaction, generate more hydration products such as calcium silicate hydrate (C–S–H), enhance the interfacial adhesion between the matrix and the aggregate, and form a closer interfacial transition zone. Moreover, the addition of NS also reduces the cumulative pore volume in concrete, refines the pore size, and makes the internal structure of concrete denser.