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• Cadmium soil pollution and crop accumulation are detectable on national level in China. • Mining activities and sewage irrigation dominate to Cd pollution in China. • Cd pollution in Southwest of China, Middle Yellow River region and North China plain should be taken more seriously. • Cd enrichment models differ with investigated sites and are influenced by pollution sources. Cadmium (Cd) pollution of agricultural soil is of public concern due to its high potential toxicity and mobility. This study aimed to reveal the risk of Cd accumulation in soil and wheat/maize systems, with a specific focus on the source-specific ecological risk, human health risk and Cd enrichment model. For this we investigated more than 6100 paired soil and grain samples with 216 datasets including soil Cd contents, soil pH and grain Cd contents of 85 sites from China. The results showed that mining activities, sewage irrigation, industrial activities and agricultural practices were the critical factors causing Cd accumulation in wheat and maize cultivated sites. Thereinto, mining activities contributed to a higher Cd accumulation risk in the southwest China and Middle Yellow River regions; sewage irrigation influenced the Cd accumulation in the North China Plain. In addition, the investigated sites were classified into different categories by comparing their soil and grain Cd contents with the Chinese soil screening values and food safety values, respectively. Cd enrichment models were developed to predict the Cd levels in wheat and maize grains. The results showed that the models exhibited a good performance for predicting the grain Cd contents among safe and warning sites of wheat (R2 = 0.61 and 0.72, respectively); while the well-fitted model for maize was prone to the overestimated sites (R2 = 0.77). This study will provide national viewpoints for the risk assessments and prediction of Cd accumulation in soil and wheat/maize systems. [Display omitted] [ABSTRACT FROM AUTHOR]