Substantially anhydrous electropolishing electrolyte solutions. The substantially anhydrous electropolishing electrolyte solutions described herein do not use water as a solvent; instead, such electropolishing electrolyte solutions use anhydrous alcohols and/or glycols as a solvent. For example, an electropolishing electrolyte solution, as described herein, may include an alcohol, at least one mineral acid, and at least one water sequestering agent. Suitable examples of water sequestering agent include, but are not limited to, polyfunctional alcohols. Methods of electropolishing metal articles using such electropolishing electrolyte solutions are disclosed herein as well.