Controlling the dimensional aspect of conductive coordination polymers is currently a key scientific interest. Herein, solution‐based dimension control strategies are proposed for copper chloride thiourea (CuCl‐TU) coordination polymers that enable centimeter‐scale, 2D nanosheet formation for use as transparent electrodes. Despite the wide bandgap of CuCl‐TU polymers (4.33 eV), through polaron‐mediated electron transfer, the electrical conductivity of the 2D sheet at room temperature is able to reach 4.45 S cm−1 without intentional doping. This leads to a highly anisotropic electronic conductivity of up to the order of ≈103 differences, depending on the material orientation. Furthermore, by substituting alternative thiourea candidates, it is demonstrated that it is possible to predesign CuCl‐TU structures with the desired functionality, stability, and porosity through dimensional control. These findings provide a blueprint to design next‐generation transparent conducting materials that can operate at room temperature, thereby expanding their applicability to different fields.
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