The talk will summarize our lab’s work developing novel biomaterial platforms emerging from the integration of supramolecular chemistry, intermolecular interactions, and engineering and biofabrication principles. These systems aim to use peptides and proteins in innovative ways to transform single molecules into useful macroscopic materials such as complex biomimetic environments, hierarchical biomineralizing matrixes, and dynamic structures that can grow and self-heal. One example consists of a tuneable organic matrix with the capacity to generate materials exhibiting crystallographically aligned hydroxyapatite nanocrystals with hierarchical order up to the macroscale, be grown over large uneven areas, and exhibit high stiffness and acid resistance. Another example includes a peptide-protein system with the capacity to access different co-assembling pathways, structures, and resulting properties. In one scenario, the system is capable of accessing non-equilibrium for substantial periods of time enabling the growth of vascular-like tubular structures with a high spatio-temporal control. Other examples that aim to create functional macroscopic biomaterials based on predictable interactions at the molecular scale will be presented. These systems offer opportunities in tissue engineering, regenerative medicine, and biomimetic in vitro models.