By specifically binding with various inorganic nanomaterials through their functional groups or introducing special reactivity, the nanostructures and biofunctions of designed peptides can be enriched. This review provides a brief discussion on the design, composition, and biomedical applications of bioinspired peptide–inorganic nanomaterial hybrids. The attaching mechanisms of different peptide–inorganic nanomaterials are discussed from the viewpoint of the functional group, nanostructure, and conformational freedom. Particularly, the structures and functions of the obtained hybrids based on different nanomaterials are described in detail. In addition, we highlight some examples of self-assembled peptide–inorganic nanomaterial systems with relevance to biomedical applications, including biosensors, cell targeting, bioimaging, biomineralization, biocatalysts, and drug delivery. We also give a short outlook on the broad prospects of the fabrication and applications of peptide–inorganic nanomaterial hybrids.