The present invention relates to surface roughening methods and more particularly to a method for electrochemical roughening of thin film macro- and micro-electrodes. In one embodiment, an electrochemical etch template is formed comprising polymer particles adsorbed on a surface of a substrate to be roughened, followed by electrochemically etching of exposed regions of the substrate between the polymer particles in the electrochemical etch template so as to selectively roughen the surface of the substrate. In another embodiment, a surface of the electrode is immersed in either a adsorbing acidic solution, such as sulfuric acid, or a non-adsorbing acidic solution, such as perchloric acid, followed by electrochemically pulse etching the surface of the substrate at a narrow frequency range for adsorbing acidic solutions, or at a wide frequency range for non-adsorbing acidic solutions.

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