The efficient hydrogenation of 1-butene is an industrially significant reaction for producing fuels and value-added chemicals. However, achieving high catalytic efficiency and stability remains challenging, particularly for cost-effective materials, such as Ni. In this study, we developed a porous Ni-coated Ni foam catalyst by electrostatic spray deposition to address these challenges. The catalyst exhibited a turnover frequency approximately 10 times higher than that of either porous Ni or Ni foam alone. This enhancement was attributed to the formation of interfacial active sites, which facilitated improved reactant adsorption and activation during hydrogenation. The electrostatic spray deposition technique ensured a uniform and controlled coating, enabling precise engineering of the catalyst structure and interface. The post-deposition heat treatment was further optimized to enhance structural integrity and catalytic performance. This study highlights the importance of interface engineering and structural optimization in catalyst design and provides valuable insights into the development of efficient Ni-based catalysts for industrial hydrogenation applications. These findings emphasize the potential of electrostatic spray deposition as a versatile method for fabricating advanced catalytic systems.