The necessity for efficient green energy production compels scientists to develop advanced nanostructured metallic alloys with tunable properties. This contribution places emphasis on tuning pore architecture and film thickness of mesoporous Pd – Cu – Si thin films sputtered on Si substrates for enhanced electrocatalytic and hydrogen sorption/desorption activity and their comparison with the state-of-the-art electrocatalysts. The small Tafel slope of 44 mV dec–1 with a rapid rise in the cathodic current rendering low hydrogen overpotentials of 24 mV at 10 mA cm–2, and the largest sorption/desorption peaks for the T4H2 electrode suggest its use for a fuel cell electrode. Moreover, the kinetic parameters described by the equivalent circuit model have a very good correlation with Tafel slopes and sample mass. The 10 nm T1H1 sample has one of the highest capacitive responses where the hydrogen-metal interaction takes place and is promising as a nano-charger and sensing of hydrogen.