The present paper reports a novel approach for fabrication of eco-friendly ZnO nanoparticles onto three-dimensional (3D)-printed polylactic acid (PLA) scaffolds/structures. Several alcohol-based traditional Greek liquors were used to achieve the corrosion of metallic zinc collected from a typical galvanic anode to obtain photocatalytic active nanostructured ZnO, varying from water, to Greek “ouzo” and “raki”, and pure ethanol, in combination with “Baker’s ammonia” (ammonium bicarbonate), sold worldwide in every food store. The photocatalytic active ZnO nanostructures onto three-dimensional (3D)-printed PLA scaffolds were used to achieve the degradation of 50 ppm paracetamol in water, under UV irradiation. This study provides evidence that following the proposed low-cost, eco-friendly routes for the fabrication of large-scale photocatalysts, an almost 95% degradation of 50 ppm paracetamol in water can be achieved, making the obtained 3D ZnO/PLA structures excellent candidates for real life environmental applications. This is the first literature research report on a successful attempt of using this approach for the engineering of low-cost photocatalytic active elements for pharmaceutical contaminants in waters.