Vacuum swing adsorption (VSA) is a promising treatment method for volatile organic compounds (VOCs). This study focuses on a VSA process for regenerating activated carbon spent with VOCs, and then investigates its adsorption capacities. Toluene was selected as the test VOC molecule, and the VSA regeneration experiments results were compared to the thermal swing adsorption process. Cyclic adsorption-desorption experiments were performed using a lab-scale apparatus with commercial activated carbon (Samchully Co.). The VSA regeneration was performed in air (0.5 L/min) at 363.15 K and 13,332 Pa. The comparative results depicted that in terms of VSA regeneration, it was found that after the fifth regeneration, about a 90% regeneration ratio was maintained. These experiments thus confirm that the VSA regeneration process has good recovery while operating at low temperatures (363.15 K) and 13,332 Pa.