Sol−gel-based carbon xerogels possess very promising properties for pollution abatement, using processes that associate adsorption and on-site electrochemical oxidation. However, combining a high exterior surface area (for efficient diffusion) and a monolithic shape (necessary for electrochemical processes) poses challenges. In this work, the shape of monolithic carbon xerogels was contrived by the use of 3D-printed molds. Several parameters were optimized: the choice of mold design, the choice of plastic, the 3D printer parameters, the solvent, and the process of dissolving the plastic. A design combining fine sticks and plates made of ABS was printed; a sol−gel carbon xerogel monolith was synthesized in it, and the mold was removed by using a combination of acetone and pyrolysis. Dissolving the plastic could be carried out by placing the material on a metallic net and leaving the dissolved ABS to settle. The resulting carbon material exhibits a high exterior surface area and good strength, leading to potential uses in the aforementioned process. The research shows that 3D printing is an efficient method of parameter optimization in pre-industrialization research, thanks to its flexibility, low cost, and ease of use.