Pervaporation is an energy-efficient membrane-based separation process that effectively separates azeotropic mixtures without requiring additives. Hydrophilic membranes are particularly suitable for ethanol dehydration. This study explores the pervaporation-dehydration of ethanol using a carrageenan-chitosan composite membrane supported by polyethersulfone (PES) and crosslinked with glutaraldehyde. The membrane’s hydrophilicity enables selective water permeation, which is evaluated through swelling degree measurements. Results indicate that membranes without chitosan exhibit the highest swelling degree, while increasing chitosan content reduces swelling. Scanning electron microscopy (SEM) reveals distinct structural differences between the carrageenan-chitosan layer and the PES support, with crosslinked membranes displaying compact bonding between layers. Optimal pervaporation performance was achieved with a carrageenan-to-chitosan ratio of 1:1, a glutaraldehyde concentration of 1%, and an immersion time of 2 hours.