Ultrathin metal-organic framework (MOF) nanosheets (NSs) offer potential for many applications,b ut the synthetic strategies are largely limited to top-down, low-yield exfoliation methods.H erein, Ni-M-MOF (M = Fe,A l, Co, Mn, Zn, and Cd) NSs are reported with at hickness of only several atomic layers,p repared by al arge-scale,b ottom-up solvothermal method. The solvent mixture of N,N-dimethylacetamide and water playskey role in controlling the formation of these two-dimensional MOF NSs.T he MOF NSs can be directly used as efficient electrocatalysts for the oxygen evolution reaction, in which the Ni-Fe-MOF NSs deliver ac urrent density of 10 mA cm À2 at al ow overpotential of 221 mV with asmall Tafel slope of 56.0 mV dec À1 ,and exhibit excellent stability for at least 20 hw ithout obvious activity decay. Density functional theory calculations on the energy barriers for OER occurring at different metal sites confirm that Fe is the active site for OER at Ni-Fe-MOF NSs.Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.