The rapid expansion of industrial activities and urbanization has exacerbated environmental and water pollution. Solar water evaporation is a promising technique for water purification. Herein, an innovative dual-functional hydrogel that combines photothermal conversion with photocatalytic degradation was successfully prepared. The composited hydrogel (MF/CNTs-1) achieves a high-water evaporation rate of 2.23 kg·m−2·h−1 under 1 sun irradiation. Furthermore, two-dimensional MgFe nanosheets synthesized via alkali etching of vermiculite can generate highly reactive radicals through photo-Fenton reaction, facilitating efficient pollutants degradation. This dual-functional evaporator harnesses solar energy to enhance both water purification and pollutant degradation, providing valuable insights into designing vermiculite-derived materials for comprehensive water treatment and sustainable water purification.