A pot experiment was carried out to study the impacts of five organic materials (rape straw, broad bean stalk, peat, pig manure compost, and biochar) on the availability of arsenic (As) and cadmium (Cd) in soil, the amount of iron plaque on the root surface, as well as the uptake and translocation of As and Cd in rice grown in an As/Cd co-contaminated yellow paddy soil. The results indicated that the application of organic materials significantly increased the contents of the soil organic matter and the yield of rice. The application of broad bean stalk, peat, pig manure compost, and biochar remarkably increased the soil pH, while the application of rape straw exerted no significant influence. The addition of organic matter reduced the available Cd content by 34.77%-82.69%. However, the effects of organic materials on the availability of As varied with the organic materials. The soil-available As content was significantly increased by the application of pig manure compost and biochar, while it was significantly decreased by adding rape straw and peat. The application of organic materials increased As and Cd contents in the Fe plaques on rice root surface by 28.49%-94.86% and 17.73%-151.03%, respectively. It also reduced the As and Cd contents in brown rice by 27.04%-82.51% and 15.87%-79.45%, respectively. The largest decrease was observed in the biochar treatment. The application of organic materials also remarkably reduced the translocation efficiency of Cd from the root-stem-leaf-grain and that of As from the stem to grain. The correlation analysis revealed that the soil pH, available Cd, and Cd content in the Fe plaques are the major factors influencing the accumulation of Cd in the rice grain. Furthermore, the soil pH, soil organic matter, and As content in the Fe plaques are the major factors influencing the accumulation of As in the rice grain. Therefore, it has been concluded that organic materials could influence the uptake and translocation of As and Cd in rice through changing the soil pH, organic matter content, and As and Cd contents in the Fe plaques.