The design of 3D monoliths provides a promising opportunity to scale the unique properties of singular carbon nanotubes to a macroscopic level. However, the synthesis of carbon nanotube monoliths is often characterized by complex procedures and additives impairing the later macroscopic properties. Here, we present a simple and efficient synthesis protocol leading to the formation of free-standing, stable, and highly conductive 3D carbon nanotube monoliths for later application in potential-controlled adsorption in aqueous systems. We synthesized monoliths displaying high tensile strength, excellent conductivity (up to 140 S m−1), and a large specific surface area (up to 177 m2 g−1). The resulting monoliths were studied as novel electrode materials for the reversible electrosorption of maleic acid. The process principle was investigated using chronoamperometry and cyclic voltammetry in a two-electrode setup. A stable electrochemical behavior was observed, and the synthesized monoliths displayed capacitive and faradaic current responses. At moderate applied overpotentials (± 500 mV vs. open circuit potential), the monolithic electrodes showed a high loading capacity (~20 µmol g−1) and reversible potential-triggered release of the analyte. Our results demonstrate that carbon nanotube monoliths can be used as novel electrode material to control the adsorption of small organic molecules onto charged surfaces.