High-strength steels are widely used in various mechanical production and construction industries for their low cost, high strength and high toughness. Among these, bainitic steels have better comprehensive performance relative to martensite and ferrite. In this paper, from the point of view of its microscopic fine structure and mechanical properties, the high-carbon silicon-containing steel Fe-0.99C-1.37Si-0.44Mn-1.04Cr-0.03Ni was austenitized at high temperature after a brief isothermal treatment at 280 °C and is briefly reviewed. We have used EBSD, TEM and 3D-APT to observe a unique transformation in which high-carbon silicon-containing steels form nanostructured bainite with nanometer widths. Intriguingly, as the isothermal duration decreases, the beam bainite width becomes increasingly finer. When the beam bainite width falls below 50 nm, there is a sudden shift in defect type from the conventional edge-type dislocations to a defect characterized by the insertion of a semi-atomic surface in the opposite direction, which leads to different degrees of reduction in the micro- and macro-mechanical properties of high-carbon silicon-containing steels from 1754 MPa to 1667 MPa. This sudden change in the sub-structural properties is typical of the reverse Hall–Petch effect.