Although two-dimensional (2D) carbon materials are widely investigated, aw ell-defined 2D carbon nanosheet with an ordered mesostructure has rarely been realized. Monolayer-ordered mesoporous carbon nanosheets (OMCNS) were prepared through confinement assembly of resol and F127 in the interlayer of montmorillonite (MONT). The nanoscale distance of the interlayer space of MONT only allowthe assembly of resol and F127 in the same plane,leading to ordered mesopores perpendicular to carbon nanosheets,and favor the formation of sp 2 carbon, resulting in ahigh degree of graphitization. The mesopores on the carbon nanosheets providee fficient ion diffusion, and the high degree of graphitization provides af ast electron-transport route,e nabling OMCNS as excellent electrode materials for electric double layer capacitors.Layered materials are am ultiple and largely unexploited source of two-dimensional (2D) systems with unusual phys-ical properties,o utstanding electrical properties,a nd most importantly,u ltrahigh exposed surface area, and these features are important for aw ide range of applications. [1][2][3] Among these materials,carbon materials with 2D or pseudo-2D morphologies are of particular interest for applications such as catalysis,water/gas purification, or energy conversion/ storage,o wing to their intrinsic advantages of large specific surface area (SSA), excellent electrical conductivity,chemical inertness,a nd low cost. [4][5][6] However,t he applications of 2Dstructured carbon materials are mostly hampered by the severe aggregation, especially after processing into ac ompressed electrode,w hich cause limitations,n amely ion accessibility,diffusion, and mass transportation. [7,8] To address the aforementioned issues,m any efforts have been devoted to construct 2D carbon materials with designed structures to increase the ion-accessible surface area and to improve the ion transport efficiency. [9][10][11][12][13][14][15][16][17] Thecommonly used methods include preparing crumpled nanosheets or incorporating small dimensional nanoparticles within the nanosheets, which can generate interlayer space when being packed together; [9][10][11][12][13] however,t he curved interlayer spacer and the randomly distributed interlayer spacers will lead to acomplex and even blocked pathway for ion diffusion, reducing the ionaccessible surface area. Furthermore,the limitations of crossplane diffusivity of ions between different layers are not addressed, thus still restricting the power delivery.A nother popular strategy is to grow vertically oriented 2D nanosheets on the substrate; [14][15][16][17] although an enlarged interlayer spacing was constructed, the mass loading of 2D nanosheets per unit area is restricted, thus limiting overall charge-storage capacity.C onsequently,i ti ss till ag reat challenge to design appropriate carbon nanostructure which could provide efficient ion diffusion routes when being packed together.Zhao et al. reported at ype of 2D monolayer ordered mesoporous carbon (OMC) through controlled low c...