© 2022 Elsevier LtdHerein, carbon nanotubes (CNTs) were oxygen functionalized by irradiation with diverse radiation sources including Am-241, Sr-90, Co-60, and Na-22 for the first time to be used as the electrode material in a high-energy supercapacitor. The oxygen contents of the irradiated CNTs were fine-tuned via the energy of the radiation source. The physicochemical characterization of as-obtained CNTs was conducted by X-Ray Diffraction (XRD), Raman, and Scanning Electron Microscopy, Energy Dispersive X-Ray (SEM- EDX) analysis whereas cyclic voltammetry and galvanostatic charge-discharge techniques were performed to assess the electrochemical performance of the as-assembled symmetrical supercapacitor cells. The CNT irradiated by Am-241 radiation source offered superior specific capacitance values compared to the other irradiated CNTs thanks to its higher content of oxygen functional groups. The highest specific capacitance for CNT Am-241 sample (with 7.32% oxygen) was calculated to be 489.6 F.g−1 at a current density of 0.1 A.g−1, which was almost 2.75 fold that of non-irradiated CNT sample. The capacitance retention of as-synthesized CNT Am-241 was determined as 98.50% for the 5,000th CV cycle. The outstanding energy density of 56.90 W.h.kg−1 was achieved even at a high power density value of 9992.19 W.kg−1, comparable to the commercial batteries, will pave the way for facile fabrication of high-energy electrochemical energy storage systems based on functionalized carbon nanotubes.