Following the expiration of the patents on fused-filament-fabrication (FFF), the availability and uses of this 3D-printing technology have exploded. Several recent reports describe how conductive composites can be used with FFF printers to generate 3D-printed electrodes (3DEs) for energy storage and electrochemical analysis. As printed materials, these electrodes have very high impedance values because of the high content of insulating thermoplastic required for FFF printers. To overcome this challenge, deposition of metals or activation with harsh chemicals has previously been employed. Here, a benign postprinting process was developed using the electrolysis of water to selectively remove the insulating thermoplastic (polylactic acid) via saponification. Optimization of the hydroxide-treatment process was found to reduce the impedance of 3DEs by 3 orders of magnitude in filaments from two manufacturers. This electrolysis-activation strategy offers a safe, accessible, and affordable means for improving the electrochemical performance of 3DEs. Here, the ability of these modified 3DEs to be used for electrochemical analysis and integrated into complex electrochemical cells is demonstrated.