Silk is a supramolecular material with exceptional properties such as mechanical robustness and biocompatibility. Here, we present a mild and substrate-independent process that leverages the self-assembly of silk protein dissolved in aqueous solution into insoluble thin-film coatings. We demonstrate that the kinetics of this process can be tuned using one or more kosmotropic factors, such as heat or potassium phosphate. Using multi-scale imaging and spectroscopy techniques, we show that these coatings can exhibit homogeneity across a large surface area and excellent fidelity to fine substrate topology. Furthermore, our studies suggest that these nano-thin coatings resist bacterial colonization and biofilm formation and are therefore promising materials for biomedical device interfaces.