The article discusses the challenges faced by water electrolysis for hydrogen production, particularly the high overpotential in conventional OER processes. It introduces a novel Anodic-Cathodic Sequential OER (ACS-OER) process that demonstrates fast kinetics and operates at significantly lower overpotentials than conventional methods. The article delves into the molecular mechanism of the ACS-OER process using advanced techniques like in situ differential electrochemical mass spectrometry and electrochemical Raman spectroscopy combined with density functional theory calculations. Results show that the ACS-OER process involves the formation of NiOO– active species through the electrooxidation of Ni(OH)2, followed by a reductive step for O2 release due to weakened Ni-O covalency. Furthermore, the article explores the benefits of incorporating a second transition metal like Fe to enhance the ACS-OER process. The proposed hybrid energy device allows decoupled HER and OER operations at low cell voltage and room temperature, facilitating efficient energy storage. Overall, the study presents a promising approach to unlock faster and more efficient water electrolysis for hydrogen production.