A single biopolymer film rarely has a competitive edge against synthetic films. One solution is to combine several layers with different properties into multilayer structures. In this way, for example, the barrier properties of bio-based materials can be improved. In this study, the multilayer films are produced by combining three different techniques/materials: 1) dispersion coating (cellulose nanofibrils, CNF), 2) atomic layer deposition (Al2O3; aluminum oxide), and 3) extrusion coating (polyglycolic acid, PGA). Especially the CNF and PGA-containing multilayer films show promising oxygen barrier improvements at different humidities. Thin inorganic coatings are brittle and sensitive toward stresses during converting, which may limit their use in such specific multilayer structures. The developed bio-based films largely fulfill the barrier requirements of fresh food packaging.