Capacitive Deionization (CDI) is an electrochemical desalination technique based on the electrical double layer, which accumulate salts from the water stream; however, achieving higher salt adsorption for low-concentration salt is hindered due to several obstacles, such as low adsorption capacity and slow kinetics on the electrode surface. In this study, we reported a novel electrode fabrication method designed to enhance the hydrophilicity of the electrode material and activate hierarchical porosity, making a more accessible adsorption surface area. This modification enables more than 210 % improvement in salt adsorption capacity, achieving 17.5 mg g-1 in a single pass process with good stability in an 850 mg/L NaCl solution at 1.2 V, surpassing most reported carbon-based electrodes under similar operating conditions. Electrode formulation consists of Nitrogen (N) and Phosphorus (P) doped hierarchical carbon nanotubes (CNTs) network blended with additional NaCl as a green and removable template to reach higher levels of porosity. The electrochemical sorption behavior of the sample was characterized over a voltage range of –0.5 to 0.7 V. Furthermore, the electrode materials were characterized utilizing various characterization methods, including Scanning Electron Microscopy (SEM), Transmission Electron Microscopy (TEM), X-ray Diffraction (XRD), Raman Spectroscopy, Fourier Transformed Infrared (FTIR), X-ray Photoelectron Spectroscopy (XPS), and Brunauer-Emmett-Teller (BET) to explore the correlation between microstructure, morphology, and properties. Our finding reveals that not only N and P can affect adsorption, but also the novel cathode preparation method, which employs a removable NaCl templated hierarchical porous electrode, has a profound effect on the electrochemical and CDI results. This finding will open a new perspective in designing electrodes for all electrochemical systems.