Abstract: The formation of membraneless organelles (MLOs) via phase separation of proteins and nucleic acids has emerged as an essential process with which cells can maintain spatiotemporal control. Despite enormous progress in understanding the role of MLOs in biological function in the last ten years or so, the molecular details of the underlying phenomena are only beginning to emerge recently. We use computer simulations of coarse-grained and all-atom models to complement experimental studies to achieve insights into the molecular driving forces underlying biomolecular phase separation. In this talk, I’ll highlight results that demonstrate our approach’s usefulness for identifying general principles and system-specific insights into biomolecular structure and function. These results also open up new avenues for the design of biomaterials with tunable properties.