AbstractMagnetic oxide semiconductors with wide band gaps have promising spintronic applications, especially in the case of magneto-optic devices. Co-doped ZnO (ZnCoO) has been considered for these applications, but the origin of its ferromagnetism has been controversial for several decades and no substantial progress for a practical application has been made to date. In this paper, we present direct evidence of hydrogen-mediated ferromagnetism and spin polarization in the conduction band of ZnCoO. Electron density mapping reveals the formation of Co–H–Co, in agreement with theoretical predictions. Electron spin resonance measurement elucidates the ferromagnetic nature of ZnCoO by the formation of Co–H–Co. We provide evidence from magnetic circular dichroism measurements supporting the hypothesis that Co–H–Co contributes to the spin polarization of the conduction band of hydrogen-doped ZnCoO.