The ordering of molecules to well-defined nanocale objects by the process of self-assembly is the principle behind the formation of many natural and biological nanostructures. In many cases, nature uses the strategy to hybridize organic and inorganic molecules/materials in order to produce more sophisticated nanostructures with advanced functions. Self-assembled peptide nanostructures (SPNs) are organic nanomaterials that have gained increased interest during recent years. Although SPNs by themselves have great potential to be used in a wide range of applications, their functions can be diversified when the self-assembling peptides are combined with inorganic materials. For instance, self-assembly of peptides in combination with inorganic nanomaterial can provide molecular recognition function to inorganic materials. Inversely, peptide-based nanostructures can become structurally more robust and have additional physical, electrical, and photophysical properties by the hybridization. Formation of well-ordered and stable structures is important for the proper function of peptides/proteins. However, peptides self-assembled in the presence of inorganic nanostructures have not been able to attain the level of ordering and structural stability when compared to the hybrid nanostructures found in nature. We are creating novel strategies for fabricating hybrid materials coated with multiple and structured peptides. The peptide-inorganic biohybrids can become smart, responsive, and adaptable materials that can sense and control diverse biological events.