This study investigates the low-temperature hydrogen plasma treatment approach for the improvement of hydrogen generation through waste aluminum (Al) reactions with water and electricity generation via proton-exchange membrane fuel cell (PEM FC). Waste Al scraps were subjected to ball milling and treated using two different low-temperature plasma regimes: Diode and magnetron-initiated plasma treatment. Hydrolysis experiments were conducted using powders with different treatments, varying molarities, and reaction temperatures to assess hydrogen generation, reaction kinetics, and activation energy. The results indicate that magnetron-initiated plasma treatment significantly enhances the hydrolysis reaction kinetics compared to untreated powders or those treated with diode-generated plasma. Analysis of chemical bonds revealed that magnetron-initiated hydrogen plasma treatment takes advantage by promoting a dual procedure: Surface cleaning and Al nanocluster deposition on top of Al powders. Moreover, it was modeled that such H2 plasma could penetrate up to 150 Å depth. Meanwhile, electricity generation tests demonstrate that only 0.2 g of treated Al powder can generate approximately 1 V for over 300 s under a constant 2.5 Ω load and 1.5 V for 2700 s with a spinning fan.