In this study, the effect of adding nano-silica (NS) particles on the properties of concrete containing coal fly ash were explored, including the mechanical properties, impact resistance, chloride penetration resistance, and freezing–thawing resistance. The NS particles were added into the concrete at 1%, 2%, 3%, 4%, and 5% of the binder weight. The behavior under an impact load was measured using a drop weight impact method, and the number of blows and impact energy difference was used to assess the impact resistance of the specimens. The durability of the concrete includes its chloride penetration and freezing–thawing resistance; these were calculated based on the chloride diffusion coefficient and relative dynamic elastic modulus (RDEM) of the samples after the freezing–thawing cycles, respectively. The experimental results showed that the addition of NS can considerably improve the mechanical properties of concrete, along with its freezing–thawing resistance and chloride penetration resistance. When NS particles were added at different replacement levels, the compressive, flexural, and splitting tensile strengths of the specimens were increased by 15.5%, 27.3%, and 19%, respectively, as compared with a control concrete. The addition of NS enhanced the impact resistance of the concrete, although the brittleness characteristics of the concrete did not change. When the content of the NS particles was 2%, the number of first crack impacts reached a maximum of 37, 23.3% higher compared with the control concrete. Simultaneously, the chloride penetration resistance and freezing–thawing resistance of the samples increased dramatically. The optimal level of cement replacement by NS in concrete for achieving the best impact resistance and durability was 2–3 wt%. It was found that when the percentage of the NS in the cement paste was excessively high, the improvement from adding NS to the properties of the concrete were reduced, and could even lead to negative impacts on the impact resistance and durability of the concrete.