The deformation of tempered martensitic structures, namely tempforming treatments, were applied to a 0.6C–2Si–1Cr steel at 500, 600 and 700°C using multi-pass caliber-rolling with an accumulated area reduction of 80%. The tensile and Charpy impact properties were investigated to make clear the relation between the microstructure and the delamination behavior of the tempformed (TF) samples. The tempforming treatments resulted in the evolution of ultrafine grain structures with strong ‹110›//rolling direction (RD) fiber deformation textures and fine spheroidized cementite particles distributions. In contrast to the ductile-to-brittle transition of the conventional quenched and tempered (QT) samples, the TF samples exhibited inverse temperature dependences of the impact toughness due to the delaminations, where the cracks branched in the longitudinal direction (//RD) of the impact test bars. As a result, high strength with excellent toughness was achieved in the TF samples. A yield strength of 1364 MPa and a V-notch Charpy absorbed energy of 125 J were obtained at room temperature in the sample that was tempformed at 500°C. The delamination was shown to occur due to the microstructural anisotropy of the TF samples, and the dominating factors controlling the delamination toughening were the transverse grain size, the grain shape and the ‹110›//RD fiber deformation texture. The discussion also indicated that the ultra refinement of the transverse grain structure was the key to enhancing both the yield strength and the toughness of the TF steel while lowering the ductile-to-brittle transition temperature.