Nowadays, tissue engineering (TE) is experiencing an increasing growth in the biomedical field. In this context, 3D printing techniques represent a powerful tool to design multi-layered structs with improved mimicry potential of the native host tissue. However, these techniques require ad-hoc engineered biomaterials to satisfy specific technological parameters in addition to biocompatibility and bioactivity. Thermoplastic poly(urethane)s (PUs) can be interesting candidates in this sense, because their building blocks can be ad-hoc selected to regulate their mechanical and thermal properties. Moreover, to improve cell adhesion and biomimicry capability, these materials can also be surface functionalized with common, eco-friendly techniques such as plasma treatment and carbodiimide chemistry.