The results of the influence of a range of process liquids on the formation of strengthened nanocrystalline structures in the surface layers of steel samples with different carbon content during thermo-deformation treatment are presented. The liquids were mineral oil; mineral oil with active additives containing polymers; water; and an aqueous solution of mineral salts based on magnesium and calcium chlorides. The thickness and hardness of the nanocrystalline layer increased with increasing steel carbon content. The thickness and microhardness of Steel C45 are 230–240 μm and 8.6 GPa, respectively, when using mineral oil with AAP, 110–120 μm and 7.2 GPa, respectively, when using mineral oil alone, and for steel CT80 when using mineral oil, they are 180–200 μm and 9.1 GPa, respectively (C45 and CT80 refers to engineering steels). The process liquid is decomposed into its component chemical elements by the high temperatures and pressures in the contact zone of the tool with the treated surface. It also gives off active hydrogen, which diffuses into the surface layer of the metal and significantly affects its formation. It was established that the greatest thickness and hardness of the layers were obtained after processing pre-hydrogenated samples. The choice of process fluid is critical during thermo-deformation treatment.