In this study, every effort was exerted to determine and accumulate data to correlate microstructural and compositional elements in ultra-low-carbon (ULC) steels to variation of carbon content (12–44 ppm), manganese (0.18–0.36%), and sulfur (0.0066–0.001%). Quantitative analysis of the ULC steel using optical microscope, scanning electron microscope, transmission electron microscope, and three-dimensional atom probe revealed the decrease of grain size and dislocation density with the increase of carbon contents and/or increase of the final delivery temperature. For a given carbon content, the grain interior carbon concentration increases as the grain size increases.