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The objective of this paper is to investigate the effect of calcium nitrite (CN) on improving the mechanical properties and microstructures of early-frozen cement paste. Cement pastes containing 1%, 1.5%, 2%, 2.5%, and 3% CN were prepared. One batch of samples was frozen at −6 °C for 7 days and then cured at 20 °C, and the other batch of samples was directly cured at 20 °C as a control. The compressive strength, ultrasonic pulse velocity, and resistivity of all specimens at different target ages were measured under these two curing conditions. The hydration products and microstructures of typical samples were observed using XRD and scanning SEM. The results showed that the addition of 1.5% CN could promote cement hydration and enhance slurry densification, thereby increasing the compressive strength, ultrasonic pulse velocity, and electrical resistivity of the slurry, and positively affecting the early freezing resistance of the slurry. However, when the CN dosage exceeded 1.5%, the internal structure of the slurry was loose and porous due to the generation of a large amount of nitrite–AFm, which negatively affects the properties of the cement paste. In addition, the effectiveness of CN is only limited to temperature environments above −6 °C. Concrete antifreeze suitable for lower temperatures still requires further research. [ABSTRACT FROM AUTHOR]