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Nonmagnetic ZnO films were found to exhibit room temperature ferromagnetism after hydrogen annealing at elevated temperatures (100–500 °C), accompanied by (OH) bonds detection. The areal saturation magnetization Ms (∼1.1×10−5 emu cm−2) was insensitive to film thickness, suggesting surface magnetism. The attribution to OH bonds on surface was further supported when the ferromagnetism disappeared after a short immersion for 1 s in acid solution while ferromagnetism was relatively stable in basic environment. The alternative H2- and Ar-annealing can switch ferromagnetic “on” and “off” state, as the annealing under Ar atmosphere can reduce OH bond quantity significantly. First-principles calculations have further confirmed that OH-terminated ZnO surface belonging to the p31m two-dimensional space group has the lowest formation energy of −2.97 eV and a magnetic moment of 0.30 μB per OH due to unpaired magnetic moment of electrons occupying O 2p orbital. Insufficient surface OH concentration may result in antiferromagnetism and/or paramagnetism.

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