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Intelligent solar water evaporation (iSWE) was achieved with a thermally responsive and microstructured graphene/poly(N‐isopropylacrylamide) (mG/PNIPAm) membrane. As the solar intensity varies, the water evaporation is tuned through reversible transformations of microstructures reminiscent of the stomatal opening and closing of leaves. Consequently, this mG/PNIPAm membrane displays a high water evaporation rate change (ΔWER) of 1.66 kg m⁻² h⁻¹ under weak sunlight (intensity<1 sun) and a low ΔWER of 0.24 kg m⁻² h⁻¹ under intense sunlight (1 sun<intensity<2 sun). Because of the double‐layer structure with predictable shape and dynamics, the leaf‐like membrane can further autonomously modulate the water evaporation by self‐curling under intense solar irradiation in accordance with simulation results. This mG/PNIPAm membrane provides a smart material platform with self …