jats:pThe microstructure of the as-quenched plate martensite in a high-C steel 100Cr6 was characterized by means of electron microscopy and atom probe tomography. The carbon redistribution behavior was investigated at the atomic scale, which revealed the nature of the transformation dynamics influenced by carbon and other substitutional alloying elements. A model was proposed to predict the carbon redistribution at twins and dislocations in martensite, which was based on their spatial arrangements.</jats:p>