In article number 1808079, Jin Zhang, Li-Zhu Wu, and co-workers describe the first superhydrophilic graphdiyne (GDY) electrode fabricated via air plasma for water oxidation. The resultant superhydrophilic CoAl-LDH/GDY electrode shows superior oxygen evolution performance in both electrocatalytic and photoelectrocatalytic systems, which benefits from the facilitated interfacial mass/electron transportation by superhydrophilic GDY.