We describe a novel approach to prepare cellular RANEY®-type catalysts by combining additive manufacturing (AM) of a Cu–Al alloy followed by selective leaching of Al with aqueous NaOH solutions. Three-dimensional cellular geometries of Cu–70Al were fabricated by laser-metal-deposition (LMD). After activation by an optimized leaching process, highly active and selective catalytic structures for CO hydrogenation to methanol were obtained.