Up to now, an array of effective strategies, such as interfacial polymerization, [4] solvothermal growth, [5] and nanosheet assembly, [6] have been progressively developed to produce homogeneous COF-based membranes for molecular and ionic separations. Among these currently available methods, COF selective layers are either directly synthesized on porous supports or crystallized at the interface followed by transferring onto supports. Thus, the accessibility to COF membranes is substantially contingent upon the strict and rational design of the substrate properties, including pore sizes, solvent resistance, and surface functionality. [7] Moreover, due to the lack of feasible and high-efficiency methods, improving the productivity of COF membranes still faces a major challenge. Being challenged by these obstacles, it is imperative to explore innovative synthesis strategies enabling the facile and highly efficient production of COF membranes on various supports.Electrosynthesis has been widely employed as a viable approach to generating thin films on a wide range of conductive substrates. [8] It stands out among the existing film fabrication techniques mainly due to its highlighted merits including high productivity and mild operation conditions. [9] Also importantly, precise control over the film growth can be readily exerted by adjusting the electrical parameters, resulting in wellregulated film structures. [10] The implementation of growing diverse films, comprised of metal-organic frameworks (MOFs), [11] conjugated microporous polymers (CMPs), [12] hydrogen-bonded organic frameworks (HOFs), [13], etc., [14] manifestly illustrates the prominent feasibility and universality of this methodology. Electrochemical polymerization and electrophoretic deposition are the two main approaches to the preparation of separation membranes via electrosynthesis. Electrochemical polymerization relies on the electrically triggered reactions on electrodes, which start from molecular building blocks. [15] For example, Lai et al. reported the electropolymerization strategy to fabricate CMP membranes for high-precision separations. [16] Additionally, a current-driven method has been proposed for fabricating MOF membranes on inorganic and organic substrates, with significantly shortened synthesis durations of several minutes. [17] Alternatively, the electrophoretic deposition focuses on the Covalent organic frameworks (COFs) have emerged as potent material platforms for engineering advanced membranes to tackle challenging separation demands. However, the synthesis of COF membranes is currently hampered by suboptimal productivity and harsh synthesis conditions, especially for ionic COFs with perdurable charges. Herein, ionic COFs with charged nanochannels are electrically synthesized on conductive supports to rapidly construct composite membranes for charge-selective separations of small molecules. The intrinsic charging nature and strong charge intensity of ionic COFs are demonstrated to collectively dominate the membrane growth. Spo...