Excessive Cd in crop grains is toxic to humans. We conducted a field experiment to investigate the effects of intercropping on rice yield and grain Cd content as well as a pot experiment to compare the rhizosphere redox potentials of low-Cd ‘Zhuliangyou 189’ and the neighboring high-Cd ‘Changxianggu’ that mediated Cd uptake in a flooded or a ridge–furrow system. In the field experiment, Cd removal from contaminated soil in intercropping was 1.44 times higher than that in monoculture of Zhuliangyou 189. In both Zhuliangyou 189 and Changxianggu, intercropping improved the grain yield and decreased grain Cd content. In the pot experiment, Fe plaque amount was strongly and positively correlated with bulk soil Fe(II) content, root H2O2 concentration, and Fe(II)-oxidizing ability of root bacteria but negatively correlated with Fe(II)-oxidizing ability of bulk soil bacteria and root Cd content. In Zhuliangyou 189, intercropping increased root H2O2 concentration, rhizosphere redox potential, iron plaque amount but decreased Cd bioavailability, Fe(II)-oxidizing ability of bulk soil bacteria, and organ Cd content. In the flooded system, Zhuliangyou 189 showed higher bulk soil Fe(II) content than Changxianggu. In the ridge–furrow system, ridges decreased the Fe(II)-oxidizing ability of root and bulk soil bacteria, thereby decreasing Fe plaque amount and increasing organ Cd content of rice. In both monoculture and intercropping systems, rice cultivars planted on ridges showed higher Cd bioavailability and lower bulk boil Fe(II) content than those planted in furrows.