Despite the current challenges facing MOF-based supercapacitors, the crystalline and highly tuneable structures of MOFs open the door to exciting new studies that are difficult to perform with traditional carbon electrode materials to assess how electrode structure impacts supercapacitor performance. At the same time, they will enable new mechanistic studies, so that the charging mechanisms leading to improved performance can be understood. We envisage that MOF chemistry can be tuned to both gain insights into ideal electrode properties and improve overall supercapacitor performance in the following ways.