Legumes are widely used in many cropping systems because they share their nitrogen fixation products and phosphorus mobilization activities with their neighbors. In the current study, however, we showed that co-cultivation with legumes increased cadmium (Cd) contamination in the adjacent crops. Both field and mesocosm experiments indicated that legumes increased Cd levels in edible parts and shoots of four neighboring crops and five maize varieties tested, regardless of the Cd levels in the soil. This enhanced Cd accumulation in crops was attributed to root interactions that alter the rhizosphere environment. Co-cultivation with legumes reduced soil pH, which somewhat increased the exchangeable forms of Cd. Our results have demonstrated the inevitable increases in Cd levels of crops as a direct result of co-cultivation with legumes even under situations when these levels are below the permissible threshold. With this new revelation, we need to consider carefully the current cropping systems involving legumes and perhaps to re-design the current and future cropping systems in view of avoiding food contamination by Cd.