Biomaterials to be applied in biomedical applications such as regenerative medicine need to fulfill the requirements of the applications in terms of material properties (e.g. mechanical proeprties, swelling) and functions (e.g. degradability, active movements, drug release). Biopolymers such as proteins and polysaccharides are interesting starting materials for the synthesis of biomaterials, as they often have a low cytotoxicity and can offer motifs for cell adhesion. Their degradability is of relevance for temporary implants, which are e.g. applied for inducing endogenous regeneration. However, there is a high tendency for self-organization of biopolymers into preferred conformations, which has a large impact on material properties. In order to effectively tailor the properties of biopolymer-based materials, their self-organization needs to be controlled. One option to do this is the synthesis of polymer networks, e.g. by crosslinking gelatin by polyaddition using diisocyanates, or functionalization with groups capable of specific physical interactions. Thermomechanical properties of the hydrogels were investigated by rheology, tensile tests, DSC, and TGA. The material properties could be tailored by the crosslinking. This can be linked on a molecular level to the organization of polymer chains, which was studied by WAXS after synthesis and during degradation.WAXS spectra showed only a minimal helix content in the materials when performing the synthesis above 40 °C. The investigations of biomaterials has to include the proof of Non-Cytotoxicity and successful applications in vivo, for which examples will be presented.