Engineering Biomolecular Self‐Assembly at Solid–Liquid Interfaces

Abstract Biomolecular self‐assembly is a key process used by life to build functional materials from the “bottom up.” In the last few decades, bioengineering and bionanotechnology have borrowed this strategy to design and synthesize numerous biomolecular and hybrid materials with diverse architectures and properties. However, engineering biomolecular self‐assembly at solid–liquid interfaces into predesigned architectures lags the progress made in bulk solution both in practice and theory. Here, recent achievements in programming self‐assembly of peptides, proteins, and peptoids at solid–liquid interfaces are summarized and corresponding applications are described. Recent advances in the physical understandings of self‐assembly pathways obtained using in situ atomic force microscopy are also discussed. These advances will lead to novel strategies for designing biomaterials organized at and interfaced with inorganic surfaces.