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The first synergistic dual-template self-assembly approach is presented for bottom-up construction of 2D mesoporous polypyrrole nanosheets based on different supramolecular assemblies, which feature a double-layered architecture, controlled pore sizes, ultrathin thickness, and large surface area. The unique structure rends them with superior reversible discharge capability, rate performance, and stable cyclability when serving as the cathode materials for Na-ion batteries.