Tissue engineering and regenerative medicine have the potential to transform the way we treat the human body. However, the ability to recapitulate the 3D environment of tissues and cells remains a major bottleneck for the field. From mimicking the complex extracellular matrix (ECM) to positioning cells in the right place at the right time, the spatiotemporal control of cells and their environment remain crucial for tissue growth. In this talk, I will focus on our molecular design and development of dynamic hydrogels for advanced tissue engineering applications. Via (macro)molecular design and synthesis, we can control the rheological properties of hydrogels and control the cell-biomaterial interactions across stiffness and relaxation timescales using dynamic covalent and supramolecular interactions. Fine tuning and balancing these dynamic systems is paramount for their applications, and indicate the significant importance of molecular design rules for dynamic interactions in functional hydrogels. With proper control of materials properties, one can enable customizable and life-like tissue constructs with cells utilizing biofabrication approaches.