Nanoporous carbon (HNC) with a flake and nanotubular morphology and a high specific surface area is prepared by using natural halloysite nanotubes (HNTs), a low-cost and naturally available clay material with a mixture of flaky and tubular morphology. A controlled pore-filling technique is used to selectively control the porosity, morphology, and the specific surface area of the HNC. Activated nanoporous carbon (AHNC) with a high specific surface area is also prepared by using HNT together with the activation process with zinc chloride (ZnCl2). HNC exhibits flakes and tubular morphologies, which offer a high specific surface area (837 m2/g). The specific surface area of AHNC is 1646 m2/g, 74 times greater than the specific surface area of pure HNT (22.5 m2/g). These data revealed that the single-step activation combined with the nanotemplating results in creating a huge impact on the specific surface area of the HNC. Both HNC and AHNC are employed as adsorbents for CO2 adsorption at different pressures and adsorption temperatures. The CO2 adsorption capacity of AHNC is 25.7 mmol/g at 0 °C, which is found to be significantly higher than that of activated carbon (AC), mesoporous carbon (CMK-3), mesoporous carbon nitride (MCN-1), and multiwalled carbon nanotube (MWCNT). AHNC is also tested as an electroactive material and demonstrates good supercapacitance, cyclic stability, and high capacitance retention. Specific capacitance of AHNC in the aqueous electrolyte is 197 F/g at 0.3 A/g, which is higher than that of AC, MWCNT, and CMK-3. The technique adopted for the preparation of both HNC and AHNC is quite unique and simple, has the potential to replace the existing highly expensive and sophisticated mesoporous silica-based nanotemplating strategy, and could also be applied for the fabrication of series of advanced nanostructures with unique functionalities.