This study assessed the modification effects of zirconia-based nanopowder and cement contents and curing age on the mechanical properties of silty soil. The orthogonal test design was applied to derive the best combination of each influencing factor using the lateral unconfined compressive test. Two-dimensional particle flow code (PFC2D) distinct-element modeling software was also used to fit and analyze the test curves, as well as simulate the triaxial test with the derived parameters. The test results reveal the optimal combination of 20% cement, 2% zirconia-based nanopowder, and 28 d curing age. The extreme difference table was used to plot the orthogonal trend diagram, and cement content was found to be the most significant factor controlling the silty soil strength. The maximum peak stress was 2196.33 kPa under the optimum combination of factors, which could be obtained through the index estimation, and these results were experimentally verified. According to the predicted strength envelope, the cohesive force of nanopowder-cement-modified silty soil in the optimal proportion was 717.11 kPa, and the internal friction angle was 21.05°. Nano zirconium dioxide will accelerate the hydration reaction of cement, the flocculent structure produced by the hydration of cement and soil particles connected to each other, play the role of filling and anchoring, and thus increase the strength of the nano-zirconium dioxide, and the optimal dosage of nano-zirconium dioxide is 2%.