To switch to alternatives for fossil‐fuel‐based polymer materials, renewable raw materials from green resources should be utilized. Chitosan is such a material that is a strong, but workable derivative from chitin, obtained from crustaceans. However, various applications ask for specific plastic properties, such as certain flexibility, hardness and transparency. With different additives, also obtainable from green resources, chitosan‐based composites in the form of self‐supporting films, ranging from very hard and brittle to soft and flexible were successfully produced. The additives turn out to belong to one of three categories, namely linear, non‐linear, or crosslinking additives. The non‐linear additives could only be taken up to a certain relative amount, whereas the uptake of linear additives was not limited within the range of our experiments. Additives with multiple functional groups tend to crosslink chitosan even at room temperature in an acidic medium. Finally, it was shown that dissolving the chitosan in acetic acid and subsequently drying the matrix as a film results in reacetylation compared to the starting chitosan source, resulting in a harder material. With these findings, it is possible to tune the properties of chitosan‐based polymer materials, making a big step towards application of this renewable polymer within consumer goods.