The aim of this study was to explore the feasible measurement of the control of cadmium (Cd) and arsenic (As) accumulation in rice grains. A field experiment was carried out to research the effect of different treatments, including spraying silicon (Si)/selenium (Se) foliar fertilizers, the application of lime (CaO), water management (continuous flooding), and the co-application of foliar fertilizers and flooding, on Cd and As accumulation in rice grains in Guangxi Province. The results indicate that Cd accumulation in rice grains decreased under different treatments and Cd content in rice grains reached the threshold of 0.2 mg kg−1. In the single technical treatments, CaO application, flooding, spraying foliar Se fertilizer, and spraying foliar Si fertilizer decreased Cd content by 73.15%, 60.44%, 45.76%, and 36.07%, respectively. However, flooding and CaO amendment enhanced As accumulation in rice grains. The co-application of flooding and spraying foliar fertilizer can simultaneously reduce Cd and As in rice grains. In addition, they resulted in lower Cd content than the single technical treatments. Among the treatments, the lowest bioaccumulation factors of Cd and As were found after the co-application of flooding and Si foliar fertilizer, which decreased these factors by 74.02% and 22.72%, respectively. These results suggest that spraying foliar Si fertilizer combined with flooding may be a promising method to synchronously inhibit the accumulation of Cd and As in rice.