Biomolecules capable of fabricating complex nanomaterials with required functions in nature have been exploited to artificially control nanomaterial synthesis in all aspects. This tutorial review provides an overview of recent efforts in biomimetic synthesis and the relevant mechanistic studies on biomolecular specificities toward material surfaces. It starts with a discussion of the state-of-the-art progress in colloidal nanocrystal synthesis, wherein the importance of the interfacial control over nanoscale building blocks discloses the potential of exploiting biomolecular recognition properties in nanostructure synthesis. Continued discussions will review the progress in biomimetic syntheses of different classes of nanoscale materials. In vitro biomimetic syntheses with both biomolecules isolated from organisms and material-specific peptide sequences selected from combinatorial molecular evolution processes will be demonstrated. The final part of the review presents the recent research efforts and advances in understanding biomolecule–inorganic material interactions. It is believed that with continued experimental efforts and fundamental understanding of biomolecule–material interactions scientists can one day harvest the ability to rationally design molecules to produce intricate material structures with a similar level of sophistication, precision, and superior functions as those found in nature.