The nanostructure and the carbon distribution in a pearlitic steel processed by torsion under high pressure was investigated by three-dimensional atom probe. In the early stage of deformation (shear strain of 62), off-stoichiometry cementite was analysed close to interphase boundaries and a strong segregation of carbon atoms along dislocation cell boundaries was observed in the ferrite. At a shear strain of 300, only few nanoscaled off-stoichiometry cementite particles remain and a nanoscaled equiaxed grain structure with a grain size of about 20 nm was revealed. 3D-AP data clearly point out a strong segregation of carbon atoms along grain boundaries. The influence of this carbon atom segregation on the nanostructure formation is discussed and a scenario accounting for the nanocrystallisation during severe plastic deformation is proposed.