Carbon aerogel fiber-paper based electrodes were subjected to nitric acid treatment and gold deposition in this study of capacitive deionization (CDI) experiments. The performance of each electrode was assessed based on their adsorption capacities in four different electrode-configurations (two symmetric and two asymmetric). The characterization of the electrodes was conducted following scanning electron microscopy, three-dimensional laser confocal microscopy, cyclic voltammetry and Fourier transform spectroscopy. Surface area and porosity measurements were conducted using BET isotherm analysis. The highest salt removal capacity in this study was 8.0 mg/g of NaCl in asymmetric electrodes configuration with the gold-deposited electrode used as anode and untreated/uncoated electrode used as cathode.