Sulfur-based electrodes, and associated systems and methods for their fabrication, are generally described. Certain embodiments relate to sulfur-based electrodes with smooth external surfaces. According to some embodiments, relatively large forces can be applied to compositions from which the sulfur-based electrodes are made during the fabrication process. In some such embodiments, the compositions can maintain relatively high porosities, even after the relatively large forces have been applied to them. Methods in which liquids are employed during the electrode fabrication process are also described.