Abstract: A field experiment was conducted in Xinpu New District, Zunyi City, Guizhou Province, in 2019 to explore the effects of different Sedum plumbizincicola intercropping patterns on the migration and availability of cadmium (Cd) in the soil around the roots of Capsicum annum. Five planting patterns were established: monoculture S. plumbizincicola, monoculture C. annum, stripe intercropping of C. annum with S. plumbizincicola (JZ1), cross intercropping of C. annum with S. plumbizincicola (JZ2), and mixed intercropping of C. annum with S. plumbizincicola (JZ3). Soil samples were collected around the C. annum roots at harvest, and the Cd content, soil pH, organic matter content, and contents of total and available nitrogen (N), phosphorus (P), potassium (K), and content of glomalin (GRSP) were measured and analyzed. The results showed that, compared to C. annum monoculture, the contents of acid-soluble Cd and reducible Cd in the soil around the C. annum roots effectively decreased by 39.6% and 23.9% in the cross intercropping system with S. plumbizincicola, and 41.5% and 29.0% in mixed intercropping system with S. plumbizincicola, respectively. The risks of soil Cd migration and availability were also reduced. Stripe intercropping C. annum with S. plumbizincicola had no effect on Cd mobility and availability in the soil around the C. annum root system. The Cd migration of the crossing intercropping and mixed intercropping systems decreased by 25.8% and 34.2%, respectively, and the Cd availability decreased by 11.6% and 26.9%, respectively. The stripe, cross and mixed intercropping systems did not affect the contents of Cd in oxidizable and residual states, but significantly increased the content of easily extracted GRSP in the soil by 24.5%, 39.9%, and 40.6%, respectively. Cross intercropping C. annum with S. plumbizincicola and mixed intercropping treatments also significantly increased the total soil GRSP content by 51.7% and 86.7%, respectively. Redundancy analysis showed that the importance of the soil environmental factors on soil Cd migration and availability followed the order: total extracted GRSP > available potassium > pH > easily extractable GRSP > total potassium > total phosphorus > total nitrogen > alkaline hydrolyzed nitrogen > available phosphorus > organic matter. The extractable GRSP and available potassium from the soil were the key regulatory factors affecting soil Cd migration and availability. In summary, intercropping with S. plumbizincicola significantly reduced the risks of Cd migration and availability in the soil around the C. annum roots, and the effects of cross and mixed intercropping were better than that of stripe intercropping. These results provide a theoretical basis for better usage of farmland with low to medium levels of Cd.