The increasing demand for energy, depletion of traditional energy sources, and environmental concerns have generated an energy crisis in recent years. To address this challenge, innovative and low-cost solutions have been sought, such as the use of 3D printing for decentralized hydrogen production. In this paper, we present the production of conductive filaments prepared from polylactic acid (PLA) and Carbon Black (CB), which were used for the 3D printing of electrodes. The produced materials were characterized by scanning electron microscopy, thermal analysis, and electrochemical techniques. The 3D-printed electrodes were used as substrates for CoPi electrodeposition to evaluate their performance in hydrogen production. The 3D-printed electrodes, made from filaments prepared in the laboratory, demonstrated superior electrochemical performance and hydrogen production compared to electrodes printed compared with commercial filament. The PLA@CB72R and CoPi#PLA@CB72R electrodes showed better hydrogen production performance, 10.08 and 10.20 μmol min−1, respectively. This study provides a perspective for the manufacture of filaments and 3D-printed electrodes for energy conversion applications, such as hydrogen production.