To develop microstructure control concepts for ensuring the toughness of high-strength steel plates, basic research was conducted using ferrite single-phase steels with different amounts of C, and the effects of the states of C were investigated along with those of solute N. In this study, Fe-0.017C (mass%) alloy, wherein the state of C was changed to a solid solution, intragranular cementite, and intergranular cementite, were used for microstructural observation, Charpy testing, and fracture surface investigation. The results reveal that the toughness of the intragranular cementite steel was the best, followed by that of solute C steel and intergranular cementite steel. In intergranular cementite steel with significantly inferior toughness, the coarse intergranular cementite leads to dislocation pile-up, initial crack formation, and macroscopic brittle fracture. The brittle fracture of intragranular cementite steel was caused by the deformation twins. It is thought that the fine intragranular cementite only had a minor effect on the crack initiation and dislocation mobility. Twin was also confirmed at the initiation point of brittle fracture in the solute C steel. Hence, it was deduced that the deterioration of toughness caused by solute C resulted from the promotion of twinning, which replaced the dislocation movements. However, the deterioration of toughness caused by solute C was smaller compared with that caused by solute N, which partly caused intergranular fracture. This is attributed to the suppression of intergranular fracture by the presence of a small amount of solute C.