Oxidation of alginate is a promising method that creates aldehyde groups, which can form stable cross-links with amine groups on chitosan. In this work, it is shown that a systematic variation in the oxidation degree of alginate dialdehyde allows for effective tuning of the swelling capacity of chitosan/alginate dialdehyde multilayer films. Furthermore, it is demonstrated that the pH-responsiveness of the multilayer films can be regulated by the choice of pH at which the layer-by-layer assembly is conducted. The combination of these two parameters allows for the designing polysaccharide multilayer films with a tunable degree of swelling and stimuli-responsiveness.