Ultrathin 2D porous carbon‐based materials offer numerous fascinating electrical, catalytic, and mechanical properties, which hold great promise in various applications. However, it remains a formidable challenge to fabricate these materials with tunable morphology and composition by a simple synthesis strategy. Here, a facile one‐step self‐flowering method without purification and harsh conditions is reported for large‐scale fabrication of high‐quality ultrathin (≈1.5 nm) N‐doped porous carbon nanosheets (NPC) and their composites. It is demonstrated that the layered tannic/oxamide (TA/oxamide) hybrid is spontaneously blown, exfoliated, bloomed, in situ pore‐formed, and aromatized during pyrolysis to form flower‐like aggregated NPC. This universal one‐step self‐flowering system is compatible with various precursors to construct multiscale NPC‐based composites (Ru@NPC, ZnO@NPC, MoS2@NPC, Co@NPC, rGO@NPC, etc.). Notably, the programmable architecture enables NPC‐based materials with excellent multifunctional performances, such as microwave absorption and hydrogen evolution. This work provides a facile, universal, scalable, and eco‐friendly avenue to fabricate functional ultrathin porous carbon‐based materials with programmability.
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