Packaging plays a critical role in ensuring food safety and shelf life by protecting against e.g., moisture, gases, and light. Polyethylene (PE) is widely used in food packaging, but it is mainly produced from non-renewable resources and it is an inefficient oxygen and light barrier. In this study, the layer-by-layer (LbL) assembly of a sustainably produced lignin-based polymer (EH) with polyethylenimine (PEI) or chitosan (CH) was used to fabricate (partially or fully) bio-based coatings with the aim of improving barrier properties of PE films. The charge density of EH was calculated using a polyelectrolyte titration method and the hydrodynamic diameters of EH, PEI and CH were determined by Dynamic Light Scattering (DLS). LbL assembly was monitored in situ via Quartz Crystal Microbalance with Dissipation (QCM-D) and Stagnation Point Adsorption Reflectometry (SPAR). PE films were coated with a variable number of PEI/EH or CH/EH bilayers (BL) using an immersive LbL assembly method. Coated films were studied in terms of light-blocking ability, wettability, thermal behaviour, surface structure, as well as oxygen and water vapor barrier properties. QCM-D and SPAR data showed a stepwise multilayer formation and strong interactions between the oppositely charged polymers, with PEI/EH coating having a greater amount of deposited polymer compared to CH/EH coating at the same number of BL. Overall, light barrier properties and wettability of the coated films increased with the number of deposited bilayers. Coated PE films maintained the overall thermal behaviour of PE. A number of BL of 20 was found to be the most promising based on the studied properties. Selected samples showed improved oxygen and water vapor barrier properties, with PEI/EH coating performing better than CH/EH coating. Taken altogether, we demonstrated that a novel and sustainable lignin-based polymer can be combined with PEI or CH to fabricate (partially or fully) bio-based coatings for food packaging.