Edible coatings attract interest today as efficient and safe techniques for controlling the deterioration andextending the shelf-lifeof food products. In the present study, a Layer-by-Layer (LbL) electrostatic deposition of oppositely charged natural polysaccharides, a polyanion alginate and a polycation chitosan, was implemented for coating a model food: fresh-cut melon. The performance of the alginate-chitosan coating was compared with single-layer coatings and with non-coated control. The LbL coating was found to possess the beneficial properties of both ingredients, combining good adhesion to melon matrix of the inner alginate layer with antimicrobial activity of the outer chitosan layer. The bilayer coating slowed down tissue texture degradation. An unexpected benefit of the LbL coating was that its enhanced gas-exchange properties exceeded those of both monolayer coatings and even of the non-coated control. As a result, the LbL coating prevented an increase in headspace CO2, ethanol, and acetaldehyde concentrations, which are the signs of hypoxic stress and off-flavor development observed in other samples, especially in alginate-coated melons. The phenomenon was presumably related to swelling behavior of the chitosan layer in the humid atmosphere of the fresh-cut melon package, giving the melon pieces an attractive succulent appearance. At the same time, the LbL coating resulted in somewhat increased produce weight loss due to the reduced surface water vapor resistance.