Two sorts of tablets were manufactured from ball-milled powder (aluminum scrap and copper) by cold pressing and spark plasma sintering. Their microstructure, phase, and elemental compositions were investigated via scanning electron microscopy, X-ray diffraction analysis, and energy-dispersive X-ray spectroscopy. New phases, Al2Cu and MgCuAl2, were detected in the samples. Their microstructure was formed by welded scrap particles, the intermetallides, and Cu-rich regions located majorly along ‘interparticle boundaries’ and, to a lesser extent, within small, micro- and nanosized ‘intraparticle spots’. The tablets were sealed with adhesive, so only the top surface was exposed to the environment, and tested in a chlorine aqueous solution for hydrogen generation performance. For both sample sorts, hydrogen yields of nearly 100% were achieved. The sintered tablets reacted faster than the cold-pressed ones: at 60, 70, and 80 °C, their entire ‘conversion into hydrogen’ took ~80, 40, and 30 min. vs. ~220, 100, and 70 min. The experimental kinetic curves were fitted with a contracting geometry equation, and those for the sintered samples were approximated with higher precision. The key effect of the additive was to enhance hydrogen evolution through the galvanic corrosion of Al in the regions adjacent to the intermetallic inclusions and Cu-rich spots.