Biohybrid materials continue to rapidly expand as they offer to combine biological functionality with synthetic materials. In biological systems, proteins are the most versatile biomacromolecules with the various functions they perform. Recognizing this, our group has been exploring peptides as the key molecular building blocks in designing functional biohybrid materials. We design peptides with different properties ranging from self-assembly to antimicrobial properties. By adapting experimental and computational approaches combined with transparent machine learning (ML) methods, we search for the peptides that present desired function. In our approach, we expanded our predictions from single function to bifunctional peptides to control their properties at the complex materials to tissue interfaces. Biohybrid materials that incorporates antimicrobial, and mineralization properties as well as bimodal imaging properties will be given as the recent examples. Biohybrid materials design provides to couple dynamic biological functions as an integral part of the resulting material system.