AbstractDiamond-like carbon (DLC) thin films were prepared by hydrothermal electrochemical method in one-step process. The structural characterization of these films was carried out by scanning electron microscopy (SEM), Raman spectroscopy, and infrared reflectance spectroscopy (IR). It was found that there was an increased sp2 carbon content but decreased sp3 carbon and hydrogen contents with an increase in current density. The flexibility and internal stresses of the DLC films were affected by hydrogen, sp3 amorphous carbon and ordered crystalline sp2 carbon contents. The highly flexible DLC films with high sp3 carbon and hydrogen contents were prepared at a current density of 0.001 mA/cm2.