The low-temperature impact toughness of nodular cast iron can be significantly enhanced by heat treatment, and thus meet the severe service requirements in the fields of high-speed rail and power generation, etc. In order to explore the enhancement mechanism, microstructure, hardness, composition and other characteristics of as-cast and heat-treated nodular cast iron is systematically tested and compared by optical microscopy, microhardness tester, EBSD, SEM, electron probe, and impact toughness testing machine in this study. The results show that heat treatment has little effect on the morphology and size of graphite in nodular cast iron, ignores the effect on the grain size, morphology, and distribution of ferritic matrix, and has little effect on the hardness and exchange of elements, while it is meaningful to find that heat treatment brings about significant decrease in high-angle grain boundaries (HAGB) between 59° and 60°, decreasing from 10% to 3%. Therefore, the significant enhancement of low-temperature impact toughness of nodular cast iron by heat treatment may result from the obvious decrease in HAGB between 59° and 60°, instead of other reasons. From this perspective, the study can provide novel ideas for optimizing the heat treatment process of nodular cast iron.