High electrolyte resistance severely limits the response time and energy efficiency of an electric double layer capacitor electrode. Vertically oriented graphene nanosheets (VOG) having open, straight channel morphology is a new, attractive morphology with low electrolyte resistance. While CVD remains the dominant synthesis method for VOG electrodes, electrochemical exfoliation of graphite, a facile, economical and scalable method for production of loose graphene flakes, can also provide a VOG electrode. Here we show, that the conditions of electrochemical exfoliation for producing VOG morphology is substantially different from using it to produce loose graphene flakes. In particular, a low pH solution leads to a better expansion of the graphite and substantially better VOG density while a high pH solution leads to the formation of loose graphene flakes. Sulfuric acid is better than other sulfate salt-based electrolyte solutions for the synthesis of a VOG electrode. The electrolyte concentration, exfoliation time, and current density also affect the electrode capacitance. The optimal process conditions provide a VOG electrode of areal capacitance 750 mF/cm2. A capacitor consisting of two identical VOG electrodes shows a volume capacitance density of 1.56 F cm−3 higher than most of the literature values for supercapacitors.