In this study, a novel rapid solid carburizing process with a large diffusion depth using nano-diamonds(NDs) was conducted for low carbon steel. Changes of annealed NDs were obtained by Raman spectroscopy and transmission electron microscopy(TEM), and the results suggested that the NDs experience a stripping process before a special solid-reaction with surface iron atoms from steel substrate. Onionlike carbon(OLC) derived from the annealed NDs provided broken graphitic ribbons as carbon sources that accelerated the rate of adsorption and diffusion. Examination of the surface layer at equilibrium using TEM and X-ray photoelectron spectroscopy(XPS) also revealed the special state of carbon, and an ultrafine mixed phase microstructure was obtained by rapid solid-phase transformation. As a result, a surface hardened layer with ultrahigh hardness and a smooth transition region were realized. We believe that these kinds of diamond or graphitic structures with high activity states have an important influence not only on adsorption and diffusion but also on this special solid-phase transformation. In this study, a novel rapid solid carburizing process with a large diffusion depth using nano-diamonds (NDs) was conducted for low carbon steel. Changes in annealed NDs were obtained by Raman spectroscopy and transmission electron microscopy (TEM), and the results suggested suggested that the NDs experience a stripping process before a special solid-reaction with surface iron atoms from steel substrate. Onionlike carbon (OLC) derived from the annealed NDs provided broken graphitic ribbons as carbon sources that accelerated the rate of adsorption and diffusion. Examination of the surface layer at equilibrium using TEM and X-ray photoelectron spectroscopy (XPS) also revealed the special state of carbon, and an ultrafine mixed phase microstructure was obtained by rapid solid-phase transformation. As a result, a surface hardened layer with ultrahigh hardness and We believe that these kinds of diamond or graphitic structures with high activity states have an imp ortant influence not only on adsorption and diffusion but also on this special solid-phase transformation.