The study aimed to investigate the surface modification of biaxially oriented polypropylene (BOPP) by layer-by-layer (LbL) assembly of lysozyme (LZ) with two different polysaccharides, iota-carrageenan (IC) and gum arabic (GA), for food packaging applications. The effects of solution pH, adsorption time, elimination of intermediate drying steps were investigated. The LbL film growth was monitored up to 10 deposition steps by UV–Vis spectroscopy and in situ surface plasmon resonance (SPR). The most successful processing conditions for both types of coatings were pH 7–7 combination with intermediate drying and 20 min adsorption time. SPR pointed out a ‘dissolution/reconstruction’ mechanism in film formation. The thickness and surface morphology of the coatings were characterized by Atomic force microscopy (AFM). The surface roughnesses of LZ/IC coatings were higher than that of LZ/GA coatings indicating a denser matrix in the latter. Deposition of 5 bilayers of LZ/IC and LZ/GA on BOPP resulted in 66.15% and 56.89% reduction in oxygen transmission rate (OTR) of the film, respectively. The corresponding reductions in water vapor transmission rate (WVTR) were 28% and 33.52%, respectively. Elimination of intermediate drying steps resulted in less overall deposition, rougher surfaces, diminished oxygen and water barrier properties. The edible LbL coatings obtained in this study possess good gas barrier properties, which is very promising for their use in the preservation of fresh/fresh-cut produce in combination with modified atmosphere packaging applications. The results promise reduced use of plastic films in food packaging.