Affordable carbon composite electrodes were developed to treat low-concentrated groundwater using capacitive deionization (CDI). A carbon slurry prepared using activated carbon powder (ACP), poly(vinylidene fluoride), and N-methyl-2-pyrrolidone was employed as a casting solution to soak in a low-cost porous substrate. The surface morphology of the carbon composite electrodes was investigated using a video microscope and scanning electron microscopy. The capacitance and electrical conductivity of the carbon composite electrodes were then examined using cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS), respectively. According to the CV and EIS measurements, the capacitances and electrical conductivities of the carbon composite electrodes were in the range of 8.35–63.41 F g–1 and 0.298–0.401 S cm–1, respectively, depending on ACP contents. A CDI cell was assembled with the carbon composite electrodes instead of with electrodes and current collectors. The arsenate removal test included an investigation of the optimization of several important operating parameters, such as applied voltage and solution pH, and it achieved 98.8% removal efficiency using a 1 mg L–1 arsenate solution at a voltage of 2 V and under a pH 9 condition.