Simultaneous Activation–Exfoliation–Reassembly to Form Layered Carbon with Hierarchical Pores

Currently, the production of hierarchical 2 D layered carbon is mostly limited by low yields, laborious processing, and the high tendency for reaggregation. Hence, it is still a challenge to attain stable porous carbon structures with a well‐preserved layered structure and hierarchical pores. Here, we demonstrate a facile and simultaneous activation–exfoliation–reassembly technique to perform structural modification and pore tailoring of carbonaceous matrices conveniently. Various pore creations can be realized concurrently from in‐plane micro‐/mesopores by chemical activation, expansion of intersheet mesopores, and interconnectivity of the layered structure to form 3 D macropores. Finally, a proof‐of‐concept demonstration of the combination of hierarchical macro‐/micro‐/mesoporous layered carbon structure and TiO 2 nanosheets shows promising adsorption and catalytic properties.