The dispersion of nano‐SiO2 (NS) in cement plays a critical role in enhancing the properties of cementitious materials. In this study, the combination of ultrasonic dispersion and polycarboxylic acid water reducing agent (PCE) was used to significantly improve the dispersion of NS. The effects of ultrasonic dispersion time, NS content, and PCE content on dispersion quality were investigated, alongside their impact on mechanical properties, electrical resistivity, and frost resistance. The results demonstrated that this synergistic method optimized the dispersion of NS, leading to superior mechanical properties and frost resistance. With an ultrasonic dispersion time of 40 min, NS content of 1.0 wt.%, and PCE content of 0.75 wt.%, the cement paste achieved its optimal performance. Compared to non‐dispersed samples, compressive strength increased by 33.7%. After 75 freeze–thaw cycles, the mass loss was 2%, the relative dynamic elastic modulus was 99.15%, and the strength loss was 13.74%.