Manipulating 2D Membrane Interlayer Channels with Accelerated Mass‐Transfer Behavior to Boost Solar Desalination

Abstract The scarcity of fresh water necessitates sustainable and efficient water desalination strategies. Solar‐driven steam generation (SSG), which employs solar energy for water evaporation, has emerged as a promising approach. Graphene oxide (GO)‐based membranes possess advantages like capillary action and Marangoni effect, but their stacking defects and dead zones of flexible flakes hinders efficient water transportation, thus the evaporation rate lag behind unobstructed‐porous 3D evaporators. Therefore, fundamental mass‐transfer approach for optimizing SSG evaporators offers new horizons. Herein, a universal multi‐force‐fields‐based method is presented to regularize membrane channels, which can mechanically eliminate inherent interlayer stackings and defects. Both characterization and simulation demonstrate the effectiveness of this approach across different scales and explain the intrinsic mechanism of mass‐transfer enhancement. When combined with a structurally optimized substrate, the 4Laponite@GO‐1 achieves evaporation rate of 2.782 kg m −2 h −1 with 94.48% evaporation efficiency, which is comparable with most 3D evaporators. Moreover, the optimized membrane exhibits excellent cycling stability (10 days) and tolerance to extreme conditions (pH 1–14, salinity 1%–15%), verifies the robust structural stability of regularized channels. This optimization strategy provides simple but efficient way to enhance the SSG performance of GO‐based membranes, facilitating their extensive application in sustainable water purification technologies.