High-pressure torsion (HPT) has been used for investigating the influence of predeformation on the fracture toughness of a fully pearlitic rail steel. The use of HPT enables one to investigate changes in fracture toughness as a function of predeformation over a wide range of strain while simultaneously studying the influence of the crack plane orientation on the fracture toughness. With increasing prestrain, besides a strong increase in hardness, a pronounced anisotropy in the fracture toughness was found. Both the increase in hardness and the anisotropic fracture behavior can be attributed to the shear deformation process leading to an anisotropic composite structure on the nanometer scale.