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Polyoxometalates (POMs), as carbon-free metal-oxo-clusters with unique structural properties, are emerging water-splitting electrocatalysts. Herein, we explore the development of cobalt-containing polyoxometalate immobilized over the carbon nanotube fiber (CNTF) (Co₄POM@CNTF) towards efficient electrochemical oxygen evolution reaction (OER). CNTF serves as an excellent electron mediator and highly conductive support, while the self-activation of the part of Co₄POM through restructuring in basic media generates cobalt oxides and/or hydroxides that serve as catalytic sites for OER. A modified electrode fabricated through the drop-casting method followed by thermal treatment showed higher OER activity and enhanced stability in alkaline media. Furthermore, advanced physical characterization and electrochemical results demonstrate efficient charge transfer kinetics and high OER performance in terms of low overpotential, small Tafel slope, and good stability over an extended reaction time. The significantly high activity and stability achieved can be ascribed to the efficient electron transfer and highly electrochemically active surface area (ECSA) of the self-activated electrocatalyst immobilized over the highly conductive CNTF. This research is expected to pave the way for developing POM-based electrocatalysts for oxygen electrocatalysis.