While bio-based but chemically synthesized polymers such as polylactic acid require industrial conditions for biodegradation, protein-based materials are home compostable and show high potential for disposable products that are not collected. However, so far, such materials lack in their mechanical properties to reach the requirements for, e.g., packaging applications. Relevant measures for such a modification of protein-based materials are plasticization and cross-linking; the former increasing the elasticity and the latter the tensile strength of the polymer matrix. The assessment shows that compared to other polymers, the major bottleneck of proteins is their complex structure, which can, if developed accordingly, be used to design materials with desired functional properties. Chemicals can act as cross-linkers but require controlled reaction conditions. Physical methods such as heat curing and radiation show higher effectiveness but are not easy to control and can even damage the polymer backbone. Concerning plasticization, effectiveness and compatibility follow opposite trends due to weak interactions between the plasticizer and the protein. Internal plasticization by covalent bonding surpasses these limitations but requires further research specific for each protein. In addition, synergistic approaches, where different plasticization/cross-linking methods are combined, have shown high potential and emphasize the complexity in the design of the polymer matrix.