The scientific community is increasingly concerned about the presence of pharmaceuticals in the aquatic environment, which is a consequence of their high consumption and inefficient removal by wastewater-treatment plants. The search for an effective and sustainable tertiary treatment is therefore needed to enhance their removal. For this purpose, the combination of electrochemical and adsorption processes into three-dimensional (3D) electrochemical systems has been proposed. In this study, a 3D system was studied to remove carbamazepine, an antiepileptic, consumed in high doses and very persistent in the environment. The influences of the following parameters on its removal were evaluated: anode and cathode materials and distance between them, electrolyte (NaCl) concentration and pH, and the (carbon-based) adsorbent material used as the particulate electrode. The obtained results demonstrated that the introduction of the particulate electrode improved the removal efficiency. This can be attributed to the simultaneous occurrence of different phenomena, such as adsorption/electrosorption, electrocoagulation, oxidation, and catalytic degradation.