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A low-cost practical technology is urgently needed to minimize cadmium (Cd) pollution in rice in many parts of the world. In the present study, we elucidated the effects and mechanisms of four alkaline compound materials via field experiments in southern China. The results indicated that these two alkaline Si–rich compound materials (AF-SC, alkaline fertilizer compounded with Si–Ca mineral powder; AF-SS, AF compounded with Si–Se mineral powder) could achieve multi-objective gains by simultaneously reducing grain Cd, increasing yield and improving soil quality at a lower cost. The grain Cd content was decreased by an average of about 75% in two field sites, which even ensured safe grain production in areas with medium Cd pollution. The rice yield was increased by a range of 6.7%–21.0% for different varieties and sites. Moreover, the materials abated soil acidification with the increase of 0.36–0.62 pH units, increased the contents of available P and available Si, subsequently reducing available Cd content in soils. Structural equation model and regression analysis showed that the alkaline environment provided by the alkaline components in compound materials effectively inhibited the formation of Fe/Mn plaques on the root surface, reducing the uptake of Cd from the environment. In addition, the decrease in grain Cd was also attributed to the inhibition of Cd translocation from root to stem, mainly caused by the increase of available Si. These findings reveal that the base application of such alkaline Si–rich compound materials is a viable solution for the remediation of Cd-polluted paddy fields in south China. [Display omitted] • Si–rich materials enable effective and low-cost remediation of Cd-polluted soils. • They also have advantages of increasing yield and improving soil quality. • Decrease of available Cd and Fe/Mn plaque caused by raised pH inhibited Cd uptake. • Increased available Si inhibited Cd transport from root to stem, further reducing grain Cd accumulation. [ABSTRACT FROM AUTHOR]