Ecological stoichiometry (ES) is an important index that reflects the balance of various elements in ecological processes. Therefore, it is of great significance to understand the soil nutrient cycle to clarify the environmental control of soil carbon (C), nitrogen (N), phosphorus (P), and potassium (K). In this study, we analyzed the spatial distribution of soil C, N, P, and K contents and the C:N:P:K stoichiometric characteristics of 0–20 cm and 20–40 cm of farmland and grassland in four agro-pastoral areas in Inner Mongolia. Spearman correlation was used to analyze the effects of environmental factors on the soil C:N:P:K stoichiometric relationship. The results showed that there was no fixed Redfield ratio for the soil stoichiometric relationship of farmland and grassland in Inner Mongolia, and the values were 15:2:1:9 to 145:10:1:26 and 25:1:1:29 to 228:15:1:65, respectively. The stoichiometric relationships between farmland and grassland were consistent with the law of geographical and spatial heterogeneity. The ratios of C:N, C:P, C:K, N:P, and N:K showed an N distribution from west to east, while the ratio of P:K showed a V distribution. The stoichiometric relationships in grassland soil were mainly affected by soil organic carbon and total nitrogen content, while those in farmland were mainly affected by total nitrogen and total phosphorus content. The annual mean precipitation has a significant effect on stoichiometric relationships in farmland, while the annual mean temperature has a more significant effect on grassland. In conclusion, the spatial distribution difference in the soil stoichiometric relationship in the agro-pastoral ecotone of Inner Mongolia was more significant than the difference in the land use pattern. The influences of annual mean temperature and annual mean precipitation on soil ecological stoichiometry were in accordance with the geographical spatial similarity law. Compared with grassland, the stoichiometric relationship of farmland soil was greatly affected by fertilization, and farmland in this region was mainly limited by carbon and nitrogen. Thus, field management should be carried out according to local conditions. This study is of great significance as it promotes the rational utilization of land resources and the sustainable development of agriculture.