energy storage and conversion devices, [26][27][28] as outlined in recent reviews (Figure 1, left). [29] Behind these applications lie a fundamental question: how water and ion transport are controlled in the laminar structure to obtain desired selectivity. A comprehensive summary of structure-transport relation is thereby imperative to understand and optimize membrane selective performance, but is so far lacking. In such context, our review aims to fill this gap by discussing: 1) how 2D materials with specific physicochemical features are assembled into laminar membranes; 2) most importantly, how membrane structure, and its response to external impacts, can tune mass transport (herein, water and ions); 3) how these transport mechanisms translate into selectivity in applications, and into future design of high-performance laminar membranes. Unsolved problems and emerging challenges around these topics are then concluded. We note that the knowledge summarized here can also, at least partly, assist the understanding of the selective gas, liquid, and micromolecule transport through laminar membranes, which are gaining considerable attention as well. [30][31][32] Transition Metal Carbides and/or Nitrides (MXene): MXene nanosheets are etched and delaminated from parent bulk MAX to M n+1 X n T x (e.g., Ti 3 C 2 T x ), and have thus several atom sublayers. [39] While M and X are early transition metal