Biomimetic materials design holds enormous potential for the generation of technologically advanced materials by exploiting the inherently specific and programmable nature of biomolecular interactions. For example, peptides that have specific affinities for materials surfaces have been utilized to control the assembly and interfacial properties of a wide range of abiotic chemistries. The complex structure and functionality native to biomolecules enables one to envision a future in which materials properties can be controlled by designing biotic/abiotic interactions. To attain this advanced level of control, a more thorough understanding of the interfacial interactions between biomolecules and materials is required. Undertaking both extensive experimental and computational studies, we have begun to unravel the influences and effects that drive biotic-abiotic interactions. In this talk, I will cover our approaches in understanding how biomolecules interact with abiotic surfaces, to control physiochemical properties by modulating these interactions, and in developing new routes for the synthesis and assembly of functional hybrid materials.