When two beads coated by surface-mobile biopolymers are brought into contact using optical traps, we observe that interparticle forces relax as a function of contact time through polymer reorganization out of the interface. These beads may be used to engineer smart materials that can access a variety of microstructures and their emergent mechano-optical properties, simply by actuating beads functionalized with biomolecules or synthetic analogues. Contributors: Yaxin Xu, Kyu Hwan Choi, Sachit G. Nagella, Sho C. Takatori