Single-crystalline mesoporous ZnO nanosheets were prepared with a green, deep eutectic solvent based antisolvent process followed by calcination at 300 °C. The antisolvent procedure led to formation of nanosheets of a mixed composition of zinc carbonate hydroxide and ZnO, calcination of which generated the product. The product nanosheets were ultrathin with a thickness of around 10 nm and pore sizes increasing from less than 10 nm to several tens nanometers with increasing calcination time and temperature. These nanosheets exhibited excellent photocatalytic efficiencies as good as that of a commercial photocatalyst, P-25 TiO 2 in terms of photocatalytic degradation of a model pollutant, methylene blue. The success is attributable to the structural advantages of the nanosheets of being ultrathin, mesoporous, and single-crystalline.