The article introduces a novel dual-site segmentally synergistic catalysis mechanism (DSSM) for CoFeSₓ nanoclusters supported on carbon nanotubes (CNTs), termed CFS-ACs/CNT, which significantly enhances the oxygen evolution reaction (OER) performance for sustainable water oxidation. Traditional mechanisms, such as the adsorbate evolution mechanism (AEM) and lattice-oxygen-mediated mechanism (LOM), face challenges in balancing high activity and stability. The DSSM mechanism, however, effectively breaks the inherent scaling relationship between key oxygen intermediates without compromising stability. This is achieved through the synergistic interaction of Co³⁺ and Fe³⁺ sites, which facilitate the formation of Co-O-O-Fe intermediates, accelerating the release of triplet-state oxygen. The CFS-ACs/CNT catalyst demonstrates superior OER performance, with a lower overpotential (270 mV at 20 mA cm⁻²) compared to commercial IrO₂ and a remarkable stability of 633 hours without significant potential loss. The catalyst's performance is attributed to its unique spin state and electronic structure, which enhance the adsorption and desorption of oxygen intermediates. Magnetic characterization and 57Fe Mössbauer spectroscopy confirm the ferromagnetic nature of the catalyst, while XANES and EXAFS analyses reveal the electronic configurations and coordination environments of the Co and Fe sites. The study also explores the catalytic mechanism from a spin state perspective, showing that the ferromagnetic coupling of Co and Fe sites enables efficient OER by facilitating the formation of the Co-O-O-Fe intermediate. DFT calculations support this mechanism, demonstrating that the DSSM pathway has a lower energy barrier compared to the AEM pathway, making it more favorable for OER. The results highlight the importance of spin-state engineering in designing high-performance electrocatalysts for sustainable water oxidation.The article introduces a novel dual-site segmentally synergistic catalysis mechanism (DSSM) for CoFeSₓ nanoclusters supported on carbon nanotubes (CNTs), termed CFS-ACs/CNT, which significantly enhances the oxygen evolution reaction (OER) performance for sustainable water oxidation. Traditional mechanisms, such as the adsorbate evolution mechanism (AEM) and lattice-oxygen-mediated mechanism (LOM), face challenges in balancing high activity and stability. The DSSM mechanism, however, effectively breaks the inherent scaling relationship between key oxygen intermediates without compromising stability. This is achieved through the synergistic interaction of Co³⁺ and Fe³⁺ sites, which facilitate the formation of Co-O-O-Fe intermediates, accelerating the release of triplet-state oxygen. The CFS-ACs/CNT catalyst demonstrates superior OER performance, with a lower overpotential (270 mV at 20 mA cm⁻²) compared to commercial IrO₂ and a remarkable stability of 633 hours without significant potential loss. The catalyst's performance is attributed to its unique spin state and electronic structure, which enhance the adsorption and desorption of oxygen intermediates. Magnetic characterization and 57Fe Mössbauer spectroscopy confirm the ferromagnetic nature of the catalyst, while XANES and EXAFS analyses reveal the electronic configurations and coordination environments of the Co and Fe sites. The study also explores the catalytic mechanism from a spin state perspective, showing that the ferromagnetic coupling of Co and Fe sites enables efficient OER by facilitating the formation of the Co-O-O-Fe intermediate. DFT calculations support this mechanism, demonstrating that the DSSM pathway has a lower energy barrier compared to the AEM pathway, making it more favorable for OER. The results highlight the importance of spin-state engineering in designing high-performance electrocatalysts for sustainable water oxidation.