Freshwater is a scarce and vulnerable resource that has never encountered such an extensive focus on a nearly worldwide scale as it does today. Recently, it has been found that desalination powered by two-dimensional (2D) carbon materials as separation membranes has significantly reduced the operational costs and complexity but presents heavy requirements for the structural stability and separation properties of the membrane materials. Here, we combined carbon materials with promising adsorption properties and zeolites characterized by a regular pore structure to obtain a zeolite-like structured carbon membrane Zeo-C and investigated the suitability of the Zeo-C membrane for seawater desalination based on the computational-simulation-driven approach. The results of molecular dynamics (MD) simulations and density functional theory (DFT) calculations revealed that the periodic pore distribution conferred favorable structural stability and mechanical strength to the Zeo-C desalination membrane. The rejection rate of Na+ and Cl- is ensured at 100% under a pressure of 40-70 MPa, and that of Na+ could reach 97.85% even though the pressure increases to 80 MPa, exhibiting superior desalination properties. The porous nature of the zeolite-like structure and the low free energy potential barrier are conducive for reliable adsorption and homogeneous diffusion of salt ions, which facilitates the acquisition of desirable water molecule permeability and salt ion selectivity. In particular, the interlinked delocalized π-network imparts inherent metallicity to Zeo-C for self-cleaning in response to electrical stimulation, thereby extending the lifetime of the desalination membrane. These studies have greatly encouraged theoretical innovations and serve as a guiding reference for desalination materials.