Exerting molecular-level control over the interaction of peptides with materials interfaces, including nanoparticles will benefit a range of areas such as biosensing, catalysis, energy, and nano-medicine. Exploitation of materials-selective binding of biomolecules is key to success in these areas; i.e. by realizing preferential adsorption of a biomolecule onto a desired materials composition, facet or polymorph. Structural characterization of the surface-adsorbed biomolecules is essential for establishing the required structure/property relationships in these systems, but is challenging to accomplish via experimental approaches alone. In partnership with experiment, molecular simulations can bring complementary insights into the origins of this selectivity, and suggest routes to manipulating these phenomena. Our team develop and apply advanced molecular simulation techniques to investigate biomolecule/materials interfaces. I will outline our recent progress in this area and discuss our findings for bio/nano applications in e.g. sensing, catalysis and energy applications.