The application of an electrochemical method to the iron-based chalcogenide superconductors has great potentials in enhancing their properties such as the superconducting transition temperature. Unfortunately, this method has been limited to polycrystalline powders or thin film samples with a large surface area. Here, we demonstrate that the electrochemical method can be usefully applied to single-crystal devices of FeSe1−xTex superconductors by combining it with the focused ion beam (FIB) microfabrication techniques. Our results open a new route to developing the high-quality superconducting devices fabricated using layered iron-based chalcogenides, whose properties are electrochemically controlled.