Conjugated Coordination Nanosheets with Molecular Rotors for Pseudocapacitors: Nanoarchitectonics and Enhanced Performance.

High‐level pseudocapacitive materials require incorporations of significant redox regions into conductive and penetrable skeletons to enable the creation of devices capable of delivering high power for extended periods. Coordination nanosheets (CNs) are appealing materials for their high natural electrical conductivities, huge explicit surface regions, and semi‐one‐layered adjusted pore clusters. Thus, rational design of ligands and topological networks with desired electronic structure is required for the advancement in this field. Herein, we report three novel conjugated CNs (RV‐10‐M, M=Zn, Ni, and Co), by utilizing the full conjugation of the terpyridine‐attached flexible tetraphenylethylene (TPE) units as the molecular rotors at the center. We prepare binder‐free transparent nanosheets supported on Ni‐foam with outstanding pseudocapacitive properties via a hydrothermal route followed by facile exfoliation. Among three CNs, the high surface area of RV‐10‐Co facilitates fast transport of ions and electrons and could achieve a high specific capacity of 670.8 C/g (1677 F/g) at 1 A/g current density. Besides, the corresponding flexible RV‐10‐Co possesses a maximum energy density of 37.26 Wh kg −1 at a power density of 171 W kg −1 and 70 % capacitance retention even after 1000 cycles.