Hydrogen is considered to be the key element to achieving climate neutrality, leading to a massive demand for electrocatalysts. This work explores the transformation of metal waste into active and stable electrode materials for water splitting by modifying the surface through atomic deposition of platinum (Pt) and cobalt (Co). Our study finds that with the addition of only 28 μg cm⁻² of Pt and 30 μg cm⁻² of Co to metal waste, high-performance electrolysis can be achieved. We investigated discarded stainless-steel (SST), titanium (Ti), and nickel (Ni) alloys and found that they had nanotextured surfaces, consisting of 10–50 nm wide grooves, which offered an excellent platform for effective bonding of Pt or Co atoms. We demonstrate a strong synergistic relationship between the metal of the swarf surface and the metal of catalytically active centers, such that only some combinations lead to effective electrocatalysts. Furthermore, we discovered that the surface density of atomically deposited Pt or Co has a profound impact on the nanoscale morphology of the active centers, providing a mechanism for the optimization of electrocatalytic characteristics. For instance, the optimal Pt loading (28 μg cm⁻²) on Ti swarf yields 5–20 nm Pt nanoparticles within the grooves with exceptional hydrogen evolution reaction (HER) activity. Similarly, the optimal surface density of Co (30 μg cm⁻²) on Ni swarf generates ∼100 nm interlinked flakes of Co(OH)₂ with outstanding oxygen evolution reaction (OER) performance. Combining these best electrodes in a full-cell electrolyser resulted in a current density of 40 mA cm⁻² at 1.6 V vs. RHE and the rates of H₂ and O₂ production of 22.09 and 10.75 mmol min⁻¹, respectively, with 100% faradaic efficiency with no decrease in activity in 24 hours. This study opens the door to more sustainable electrode fabrication and effective hydrogen production in alkaline water electrolysis.