We report a novel strategy to render stainless steel (SS) a more versatile material that is suitable to be used as the substrate for preparing electrodes for efficient hydrogen evolution by interface engineering. Our strategy involves the growth of carbon nanotubes (CNTs) by atmospheric pressure chemical vapor deposition (APCVD) as the interface material on the surface of SS. We optimized the procedure to prepare CNTs/SS and demonstrate a higher activity of the CNTs/SS prepared at 700 °C for the hydrogen evolution reaction (HER) when compared to samples prepared at other temperatures. This can be attributed to the higher number of defects and the higher content of pyrrolic N obtained at this temperature. Our strategy offers a new approach to employ SS as a substrate for the preparation of highly efficient electrodes and has the potential to be widely used in electrochemistry.