This study investigated membrane capacitive deionization (MCDI) at a pilot-scale using ion-selective polymercoated carbon electrodes for wastewater reuse. Several issues have been addressed to verify the suitability of MCDI for wastewater reclamation: electrosorption performance, removal efficiency and selectivity of ions present in wastewater, optimization of operating conditions, and performance degradation in long-term caused by the accumulation of organic contaminants. The coated electrodes had better adsorption capacities and charge efficiencies than the conventional MCDI system, which was attributed to their low electrical resistance induced by the thin coated layer. The pilot-scale MCDI test cell involved 50 pairs of anion-and cation-selective electrodes and achieved good removal efficiency of ions from the wastewater effluent, particularly for problematic charged impurities, such as nitrate (NO3-) (up to 91.08% of NO3- was removed). Increasing the flow rate and reducing the applied potential were shown to be efficient for achieving better water quality by enhancing the NO3 selectivity. Last, the 15 d operation showed good reproducibility in electrosorption and regeneration for the coated electrodes, despite the fact that high concentrations of organics were contained in the wastewater feed solution (12.4 mg/L of dissolved organic carbon).