Electric double layer capacitors (EDLCs) are a category of supercapacitors that generally compliment the performance of batteries through delivery of high power with significantly longer cycle life. The conventional active electrode material utilized in these EDLCs is activated carbon (AC) possessing high surface area through templated porosity. However, one of the primary limitations with AC-based supercapacitors using organic electrolytes is the operational voltage maximum around 2.75 V. Operation at higher voltages that push the 2.75 V barrier is the next essential developmental breakthrough to enable significant boosts to both energy and power densities of supercapacitors. Research into alternative active electrode materials is equally critical to enable and support high voltage operation of supercapacitors. This work demonstrates the fabrication of carbon nanotube (CNT) electrodes from organic-based dispersions without the inclusion of surfactant or binder, and subsequent assembly into supercapacitor devices. The performance of pouch cells assembled from the CNT electrodes and using conventional organic electrolytes at operating voltages ≥ 2.7 V is discussed. A significant and linear voltage dependence of capacitance (~ 3 times higher than AC) was observed for cells with CNT electrodes up to operational voltages ~ 3.5 V, which are currently not achievable using AC-based cells. Repeatable charge-discharge operation of the CNT-based EDLCs was demonstrated at 3.5 V and 70°C, with consequential increase to capacitance by ~ 25 - 30 % compared to 2.7 V operation. Power and energy densities were increased by 1.5 and 2 times respectively at 3.5 V compared to operation at 2.7 V. The performance characteristics from such CNT-based pouch cells were benchmarked against commercial-grade AC supercapacitor devices using organic electrolytes and rated at 2.75 V (single cell). Long-term performance advantages were observed for the CNT-based monocells at 3.5 V and 70°C, which passed 100k cycling tests at full discharge. Under the same test conditions, commercial AC-based cells failed early during the 100k cycling. Response times approaching 2 ms (at -45° phase angle) were also demonstrated with EDLC devices using thin CNT electrodes with 1 mF capacitance. Such EDLC devices may potentially rival aluminum electrolytic capacitors (AECs) for alternating current line-filtering applications, offering significant space savings compared to the bulky AEC components. Finally, the scalable fabrication of binder-free CNT electrodes from surfactant-free dispersion of the material was demonstrated by roll-to-roll, slot-die coating onto an Al foil current collector. The processing of these conformal CNT coatings, assembly into 18650 cylindrical cells, and the resulting EDLC performance characteristics are discussed. The CNT-based 18650 cells had an average capacitance of 7 F at 2.7 V, with low average ESR of 7 mΩ at 1 kHz, and average response time of 120 ms at -45° phase angle.