The development of economical and highly efficient catalysts is a challenging task for sustainable and eco-friendly hydrogen energy utilization. Alloying non-noble metal with noble metal is considered a promising catalyst for the dehydrogenation of formic acid (FA)/sodium format (SF) systems. However, the structural complexities that arise in poly-metallic catalysts make their fabrication much more costly and complicated. So, it is of utmost importance to explore a facile and cost-effective strategy for the fabrication of a simple structured solid nano-catalyst with outstanding performance and selectivity for H2 generation without CO evolution from the FA/SF system. In the current study, a phenolic-enriched extract of wild olive leaves was employed for the synthesis of ZnO nanoparticles (ZnO@WOLE NPs). TEM analysis revealed that the size of ZnO@WOLE nanoparticles was approximately 32.50 ± 3.43 nm. Zeta potential evaluation (38.39 ±1.32 mV) demonstrated the significant stability of the nanoparticles. XRD analysis provided insights into the formation of hexagonal wurtzite phase ZnO nanoparticles. These resulting ZnONPs@WOLE show extra-ordinarily high catalytic performance and approximately 80% selectivity for H2 generation from the FA/SF system at 50 °C. A turn-over-frequency and activation energy values for dehydrogenation of FA were noted as 1519 h-1 and 32.1 kJ mol-1, respectively. Furthermore, ZnO@WOLE NPs exhibited potent antioxidant activity against, hydroxyl, DPPH, superoxide, and peroxide radicals. Moreover, the synthesized nanoparticles showed the highest seed germination of Okra seed at a concentration of 1.25 µg mL-1. Whereas, the highest shoot length and root length were observed at the concentration of 1 µg mL-1.