Processes for increasing the hardness value of steel are among the most challenging in industrial applications. SKD11 steel is one of the steels that is commonly used in industry (building, transportation facility construction, and production of various kinds of scissors such as knife-edge mold, scissors, circular saw blades, and metal stamping mold). However, SKD11 steel has a hardness value of only around 58–60 HV. Even though it is often used for building and transportation facility construction, which requires material with a high hardness performance. It will be better if the hardness performance is increased. The deposition of carbon thin films with plasma sputtering is a physical vapor deposition method that is effective for improving the hardness value of material. The purpose of this study is to obtain the maximum average hardness value of carbon thin films on SKD11 through the optimization of the argon gas flow rate parameter on plasma sputtering. The effect of the argon gas flow rate parameter on the hardness value of carbon thin films for SKD11 steel is investigated using a Vickers hardness tester. The research method involves the use of target material from battery waste (carbon rods) using argon gas low-frequency plasma sputtering with variations in the argon gas flow rate of 20, 40, 60, 80, and 100 mL/min for 2 hours at 300˚C. The method allows for the improvement of the hardness performance of carbon thin films because the argon gas flow rate affects the probability of carbon atom collision with particles in the chamber and the number of argon ions formed. This can cause different structures and hardness values of thin films. Based on the results, it can be concluded that the optimum argon gas flow rate parameter is 80 mL/min, which is associated with the highest average hardness value of 335.9 HV.