The conversion of croplands to shrublands is a common approach used to control soil erosion in the drylands of the Loess Plateau in China and affects the soil, water, and carbon cycles. Knowledge of the soil water content (SWC) and soil organic carbon (SOC) content in response to land-use change is essential for optimizing revegetation strategies and improving ecosystem services. This study investigated the distribution characteristics of the SWC and SOC content for the 0–500 cm soil layer in 11 croplands and 39 shrublands planted on a former cropland over 50 years ago. The coupled and trade-off relationship between soil water consumption and carbon fixation in the shrubland soil was also analyzed. The results showed that the SOC content and SWC of the shrublands and croplands varied with soil depth, but their distribution patterns were similar under both land-use types. Planting shrubs on slopes reduced the SWC but did not significantly enhance the SOC content, indicating that cropland-to-shrubland conversion results in excessive soil water depletion without increasing carbon fixation in the soil. Additionally, both the SOC content and SWC of the shrublands varied significantly with slope positions (p < 0.05) and showed intermediate coordination levels across the entire slope. Moreover, the SOC content provided higher benefits than SWC, where the foot slope showing a relatively higher coupling coordination degree and a lower trade-off than other slope positions. These results suggest that shrubs provide a limited contribution to improve SOC stocks in the drylands of the Loess Plateau and that reductions in deep soil water under cropland-to-shrubland conversion require consideration when planning future ecological restoration measures. To improve ecosystem services (carbon sequestration and soil conservation) without compromising water resources in the drylands of the Loess Plateau or similar regions worldwide, it is necessary to fully consider the slope position and the trade-off between the SWC and SOC content.