Despite decades of study, relatively little is yet understood regarding the molecular-level events that mediate proteinsurface interactions. Experimental methods alone are generally too limited to provide the atomistic level of detail that is needed to characterize the molecular interactions that are involved. Molecular modeling methods, on the other hand, are inherently able to provide this capability. However, these computational methods require experimental data for tuning and validation before they can be confidently applied. In order to address this 'chicken-or-the-egg' type of problem, we are working on the synergistic development of experimental methods to provide the kinds of data that are needed to both tune and validate molecular simulation methods along with simulation methods that are needed for proper comparison with experimental results. The combination of these methods paves the way towards accurate prediction of protein adsorption behavior. Once developed, these methods have the potential to provide a valuable tool to help understand, predict, and control protein-surface interactions.