The impact of various crop rotation systems on the potential for soil carbon sequestration and stoichiometric characteristics is not yet fully understood, which poses challenges for effective land management and utilization. This study selected three typical crop rotation methods in the Longzhong Loess Plateau: maize–alfalfa rotation (MA), maize–sainfoin rotation (MS), and maize–wheat rotation (MW). Soil physical and chemical indices were measured, and the soil carbon density and soil stoichiometry were calculated and analyzed. The results show that the soil C/N of the surface soils was low across the rotation methods, indicating a rapid rate of organic matter decomposition and mineralization, which may hinder soil nutrient accumulation. The soil N/P was found to be lower than the national average of 8.0, indicating that nitrogen is a limited nutrient in the soil under the three crop rotation systems in this region. The soil total nitrogen content can be increased by rotation with leguminous forage. Sainfoin rotation can enhance the soil total carbon and organic carbon content, thereby improving the soil’s carbon sequestration potential. The research findings provide a theoretical foundation for the selection of appropriate rotation methods and the maintenance of the stability of agricultural ecosystems in semi-arid regions.