This work is a comprehensive study describing the optimization of the solvent-activated carbon-based 3D printed electrodes. Three different conductive filaments were used for the preparation of 3D-printed electrodes. Electrodes treatment with organic solvents, electrochemical characterization, and finally electroanalytical application was performed in a dedicated polyamide-based cell also created using 3D printing. We have investigated the effect of the used solvent (acetone, dichloromethane, dichloroethane, acetonitrile, and tetrahydrofuran), time of activation (from immersion up to 3600 s), and the type of commercially available filament (three different options were studied, each being a formulation of a polylactic acid and conductive carbon material). We have obtained and analysed a significant amount of collected data which cover the solvent-activated carbon-based electrodes surface wettability, microscopic insights into the surface topography analysed with scanning electron microscopy and atomic force microscopy, and finally voltammetric evaluation of the obtained carbon electrodes electrochemical response. All data are tabulated, discussed, and compared to finally provide the superior activation procedure. The electroanalytical performance of the chosen electrode is discussed based on the voltammetric detection of ferrocenemethanol.