Large-particle-size graded crushed stone mixtures (LPS-GCSMs) can improve the shortcomings of conventional graded crushed stone, such as low strength, high deformation, and a low modulus of resilience. At present, there is no systematic research on the gradation design and field evaluation of the LPS-GCSMs. In this study, compaction and California bearing ratio (CBR) tests and field construction conditions were combined to design six kinds of gradation of LPS-GCSM, and the optimum gradation was revealed. In order to improve the mechanical properties of LPS-GCSM, 2.5% cement was added to the mixture to prepare a low-content cement-modified LPS-GCSM (LCC-LPS-GCSM) based on the suggested gradation. The mechanical properties of the LCC-LPS-GCSM were investigated through unconfined compression strength (UCS) and compression rebound modulus (CRM) tests. Moreover, the compaction and deflection properties of LPS-GCSM and LCC-LPS-GCSM were examined through the test battery. The results showed that the optimum gradation of LPS-GCSM can be achieved with a combination of aggregate sizes of 20–40 mm, 10–20 mm, 5–10 mm, and 0–5 mm at a ratio of 44:20:10:26. The passing rates of 19 mm and 4.75 mm should be approximately at the median value of the gradation in view of field construction uniformity and a coarse aggregate interlocking effect. The UCS and CRM values of LCC-LPS-GCSM increased rapidly from 0 day to 28 days while they slowed after 28 days, which was similar to those of cement-stabilized materials. The field detection suggested that LPS-GCSM exhibited favorable compaction and that the addition of cement improved the stability of the field compaction of the mixture. Adding a subbase course of LPS-GCSM between the old pavement and the LCC-LPS-GCSM base can lead to more uniform stress on the base. The results of this study provide a reference for the gradation design of LPS-GCSM and optimization of the design indicators.