g-C 3 N 4 membranes were modulated by intercalating molecules with SO 3 Ha nd benzene moieties between layers. The intercalation molecules break up the tightly stacking structure of g-C 3 N 4 laminates successfully and accordingly the modified g-C 3 N 4 membranes give rise to two orders magnitude higher water permeances without sacrificing the separation efficiency.T he sulfonated poly(2,6-dimethyl-1,4-phenylene oxide) (SPPO)/g-C 3 N 4 with at hickness of 350 nm presents an exceptionally high water permeance of 8867 Lh À1 m À2 bar À1 and 100 %rejection towards methyl blue,while the original g-C 3 N 4 membrane with at hickness of 226 nm only exhibits apermeance of 60 Lh À1 m À2 bar À1 .Simultaneously,SO 3 Hsites firmly anchor nitrogen with base functionality distributing onto g-C 3 N 4 through acid-base interactions.T his enables the nanochannels of g-C 3 N 4 based membranes to be stabilized in acid, basic, and also high-pressure environments for long periods.Recently,two-dimensional (2D) materials (for example, graphene, [1] metal-organic framework (MOF) nanosheets, [2] covalent organic framework (COF) nanosheets, [3] exfoliated dichalcogenides, [4] and MXenes [5] )have emerged as promising building blocks for the construction of the next-generation nanofiltration membranes.2 Dl amellar nanofiltration membranes own prominent advantages of robust stability,e asy engineering of interlayer sizes and chemistry,a nd ultrafast molecule permeances over the conventional polymer-based membranes. [6] Attributed to their unique performances, scientists have contributed considerable efforts to this newly established field. Fore xample,S hi and co-workers reported the solvated graphene membrane exhibited aw ater permeance of 90 Lh À1 m À2 bar À1 ,a nd it rejected almost 100 % molecules with sizes of above 2.6 nm. [7] Peng et al. prepared WS 2 nanosheets membranes,and gained water permeances of above 700 Lh À1 m À2 bar À1 as well as moderate rejections. [8] Currently,t he further improvement of permeation while retaining acceptable rejection is still at ough task. For2 D membranes stacking by dense sheets,their molecule transfer pathway is relatively long (hundreds of nanometers to af ew micrometers), depending on the in-plane sizes of nano-