Carbon felt (CF) is an inexpensive carbon-based material that is highly conductive and features extraordinary inherent surface area. Using such a metal-free, low-cost material for energy storage applications can benefit their practical implementation; however, only limited success has been achieved using metal-free CF for supercapacitor electrodes. This work thoroughly studies a cost-effective and simple method for activating metal-free self-supported carbon felt. As-received CF samples were first chemically modified with an acidic mixture, then put through a time optimization two-step electrochemical treatment in inorganic salts. The initial oxidative exfoliation process enhances the fiber’s surface area and ultimately introduced oxygen functional groups to the surface, whereas the subsequent reduction process substantially improved the conductivity. We achieved a 205-fold enhancement of capacitance over the as-received CF, with a maximum specific capacitance of 205 Fg−1, while using a charging current density of 23 mAg−1. Additionally, we obtained a remarkable capacitance retention of 78% upon increasing the charging current from 0.4 to 1 Ag−1. Finally, the cyclic stability reached 87% capacitance retention after 2500 cycles. These results demonstrate the potential utility of electrochemically activated CF electrodes in supercapacitor devices.