An investigation of the electrolytic polishing of copper by the Jacquet method has thrown new light on the mechanism responsible for the polishing action. From a study of the voltage‐current curves it is concluded that when conditions are right for polishing the concentration of dissolved copper at the anode is the highest possible. Accordingly the concentration gradient which exists at the anode limits the rate at which copper can dissolve,i.e., diffuse into the bulk of the electrolyte (orthophosphoric acid). Since there is greater diffusion from raised areas of the anode because of steeper concentration gradients near them, the surface will become progressively more nearly level. The surface does not etch for the concentration gradient alone controls the rate of solution. Details are given for the electrolytic polishing of iron with an orthophosphoric acid electrolyte. A convenient form of cell for electrolytic polishing is described.