Regeneration is required to restore the adsorption performance of activated carbon used as an adsorbent in water purification. Conventional thermal and electrochemical regenerations have high energy consumption and poor mineralization of pollutants, respectively. In this study, phenol-saturated activated carbon fiber was regenerated in situ using an electro-peroxymonosulfate (E-PMS) process, which mineralized the desorbed contaminants with relatively low energy consumption. The initial adsorbed phenol (81.90%) was mineralized, and only 4.07% of the initial concentration remained in the solution after 6 h of E-PMS regeneration. The phenol degradation was dominated by hydroxyl radical oxidation. Adding the PMS in three doses at 2 h intervals improves the regeneration performance from 75% to more than 82%. Regeneration retained 60% of its initial effectiveness even in the 10th cycle with 4.40% of the initial concentration of phenol remaining in the solution. These results confirm the E-PMS regeneration process as effective, sustainable, and environmentally friendly for regenerating activated carbon.