In the quest for more efficient and cost-effective electrocatalytic systems, careful selection of catalysts and substrates plays a pivotal role. This study introduces an approach by synthesizing and depositing NiFe-layered double hydroxide (NiFe-LDH) catalysts on commercial AISI 304 substrates by using a low-temperature spray-coating technique. Through systematic investigations, the influence of processing conditions, such as the synthesis, ultrasonic power for having a stable nanoparticle's dispersion, and spray cycle optimization on the electrochemical and morphological properties of the coatings, is thoroughly explored. The results showcase exceptional catalytic performance, achieving an overpotential of 230 mV at 10 mA/cm2, with enhanced stability even at high current densities of 500 mA/cm2. The study highlights the significance of meticulous processing optimization and presents a scalable methodology that holds great potential for developing catalysts for oxygen evolution reactions (OER) and facilitates their integration into industrial processes.