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The electropolishing behaviour of 73 brass was studied by means of a rotating cylinder electrode (RCE) in a 70 vol % H3PO4 solution at 27 °C. Owing to the formation of a blue Cu2+-rich layer on the brass-RCE, an obvious transition peak was detected from kinetic- to diffusion-controlled dissolution in the anodic polarisation curve. Electropolishing was conducted at the potentials located at the transition peak, the start, the middle, and the end positions in the limiting-current plateau corresponding to the anodic polarisation curve of the brass-RCE. A well-polished surface can be obtained after potentiostatic electropolishing at the middle position in the limiting-current plateau. During potentiostatic etching in the limiting-current plateau, a blue Cu2+-rich layer was formed on the brass-RCE, reducing its anodic dissolution rate and obtaining a levelled and brightened brass-RCE. Moreover, a rod climbing phenomenon of the blue Cu2+-rich layer was observed on the rotating brass-RCE. This enhances the coverage of the Cu2+-rich layer on the brass-RCE and improves its electropolishing effect obviously.