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2D soft nanomaterials are an emerging research field due to their versatile chemical structures, easily tunable properties, and broad application potential. In this study, a benzene‐bridged polypyrrole film with a large area, up to a few square centimeters, is synthesized through an interfacial polymerization approach. As‐prepared semiconductive films exhibit a bandgap of ≈2 eV and a carrier mobility of ≈1.5 cm2 V−1 s−1, inferred from time‐resolved terahertz spectroscopy. The samples are employed to fabricate in‐plane micro‐supercapacitors (MSCs) by laser scribing and exhibit an ultrahigh areal capacitance of 0.95 mF cm−2, using 1‐ethyl‐3‐methylimidazolium tetrafluoroborate ([EMIM][BF4]) as an electrolyte. Importantly, the maximum energy and power densities of the developed MSCs reach values up to 50.7 mWh cm−3 and 9.6 kW cm−3, respectively; the performance surpassing most of the 2D material‐based MSCs is reported to date. [ABSTRACT FROM AUTHOR]

2D conjugated metal–organic frameworks (2D c‐MOFs) are emerging as unique electroactive materials for electronics and spintronics. The structural design and discovery of Kagome‐type 2D c‐MOFs exhibiting a metallic state are of paramount significance, yet remain rarely explored. Here, the solution synthesis of benzenehexol‐based 2D c‐MOFs based is presented on the tetrahydroxy‐1,4‐quinone (THQ) ligand. This study shows that controlling the pH of the reaction system to ≈7.5 yields an energetically favorable nonporous Cu3(C6O6) with a Kagome lattice, while at a pH of ≈10, the known porous Cu3(C6O6)2 with a honeycomb lattice is obtained. The crystal structures of both Cu3(C6O6)2 and Cu3(C6O6) are resolved with near‐atomic precision (resolution, 1.8 Å) using an imaging technique. Unlike the p‐type semiconducting behavior of Cu3(C6O6)2, theoretical studies identify Cu3(C6O6) as a metal due to its unique structural topology. The metallic state of Cu3(C6O6) is experimentally validated by terahertz time‐domain spectroscopy (THz‐TDS), which shows an increase in conductivity upon cooling. Scattering‐type scanning near‐field optical microscopy (s‐SNOM) measurements further support these findings by revealing an increase in normalized reflectivity with decreasing temperature. This work provides a new avenue for tailoring the structural topology of 2D c‐MOFs to attain the Kagome lattice and metallic state. [ABSTRACT FROM AUTHOR]