Direct diamond deposition on a steel surface has been considered very difficult. Recently, we found that high-quality diamond films can be deposited on the surface of stainless-steel X5CrNi 18-10 by drilling multiple regularly arranged pits without interlayers or seeding. The following two hypotheses (A) and (B) can be considered as the reason why a high-quality diamond film can be deposited: (A) unoxidized Cr and Ni exposed to the stainless-steel X5CrNi 18-10 surface prevent carbon diffusion into interior of the stainless-steel, resulting diamond core generation, (B) Surface geometry with regular roughness contributes to stress relaxation and delamination prevention. In the present study, those hypotheses have been examined by quantum chemistry calculation and experimental. For the quantum chemistry calculation, energy barrier and kinetic energy for a carbon atom intrudes into a model cluster has been calculated with an ab-initio computational chemistry software package, Gaussian. The calculation result has supported hypothesis (A). For the experiment, X5CrNi 18-10 stainless-steel substrates with different surface characteristics are prepared by using various mechanical machining methods and used in the direct deposition process for diamond with in-liquid plasma CVD. The experimental result has supported both hypothesis (A) and (B).