Cd contamination in rice grains has become a topic of great concern because of the high health risks associated with the long-term consumption of Cd-contaminated rice. Identification of Cd sources in rice grains by scientific methods is important for controlling heavy metal pollution and protecting human health. Here, the Cd concentrations and Cd isotopic compositions of rice plants (root, stem, leaf, and grain) and topsoil, and possible pollution sources (agricultural fertilizers, industrial dust, and automobile exhaust) were analyzed using an instrument of inductively coupled plasma mass spectrometry (ICP-MS) and multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). The results showed variations in the Cd isotopes of different components of rice plants and the fractionation coefficient of rice grains relative to topsoil (Δ114/110Cdrice grains−topsoil = 0.25‰). The contributions of pollution sources to rice grains were realized by combining the Cd isotopic composition with an isotopic mixing model (Isosource). The analysis showed that all three possible pollution sources contributed to the Cd in the rice grains in the field, the average Cd contribution of industrial dust, agricultural fertilizers and automobile exhaust was 87%, 9%, and 4%, respectively. Our study provides a feasible method for the identification of pollution sources of Cd in rice grains at the field scale and demonstrates that Cd isotopic composition is one of the powerful tools to trace the pollution sources of Cd in crops.